TRANSPORT AND RECOMBINATION MECHANISMS IN NANOCRYSTALLINE SEMICONDUCTORS

THESIS SUBMITTED FOR THE DEGREE OF DOCTOR OF PHILOSOPHY (PHYSICS) BY

JASA RAM

under the supervision of

Prof. S.R. DHARIWAL

DEPARTMENT OF PHYSICS, JAI NARAIN VYAS UNIVERSITY JODHPUR – 342 005 INDIA 2006

Prof. S.R. Dhariwal

Phone: +91-0291-2722543 E-mail: dhariwalsr@yahoo.com , 2006

CERTIFICATE
This is to certify that the thesis entitled “TRANSPORT AND RECOMBINATION MECHANISMS IN NANOCRYSTALLINE SEMICONDUCTORS” is hereby submitted in full requirement for the degree of Doctor of Philosophy (Physics) to the Jai Narain Vyas University, Jodhpur (India). It is a record of original investigation carried out by Mr. Jasa Ram, Scientist ‘C’, DRDO, Defence Laboratory, Jodhpur during the period November 2000 to July 2006 under my supervision and guidance and he has fulfilled the conditions laid down by Jai Narain Vyas University, Jodhpur for submission of Ph.D. thesis. The work presented in the thesis has not been submitted for any other degree or diploma anywhere else in India or abroad.

Dr. S.R. Dhariwal Research Supervisor Head, Department of Physics J.N.V. University, Jodhpur

TO MY PARENTS

For their faith in my education

I acknowledge thanks to DRDO for providing the genial opportunity to continue this research work. Grateful thanks are also due to former Directors of Defence Lab Dr. Defence Laboratory. Tripathi. Ojha and Shri Tulja Shanker Shrimali for all the cooperation and moral support during the progress of the work.) Prem Lata Dhariwal for her gratifying compassion in sparing sir’s time for this research work during holidays and even before & after office hours. scholarly advice and constant encouragement have abundantly helped me in this endeavor. Nevertheless.K. NRMA Division of Defence Lab for his support. Bhatnagar. His purposefulness.L. passionate interest.R. Shri L. I am also thankful to Shri D. Head.P.N.R. Baheti.K. B. Gupta and Prof. J. Jodhpur under whose able supervision and expert guidance. Mr. Shri V. Shri Gumana Ram.V. I express grateful thanks to Madam Dr. Dr. I record my grateful thanks to Dr. profound regard and indebtness to my erudite research supervisor Prof. Faculty of Science. Meena for their encouragement. Tripathi. M.K. Syal for their kind gesture of according permission to carry out the work. S. Ravindra. this thesis work has been carried out. Ram Gopal and Shri R. (Mrs. Shri K. Songra. in-depth involvement. Director. Chacharkar. V. Head. I avail this opportunity to express my sincere. Dhariwal for their support during the research . Kumar. Shri Nisheet Saxena. suggestions and fruitful discussions. Meghwal. Dhariwal. Bhandari.R.P. I hearty express my sincere gratitude to Prof. I extend my sincere thanks to Shri G. constructive criticism. Jodhpur for resolute inspiration and keen interest in the present work. Additional Director of Defence Lab for their valuable suggestions.C. Department of Physics and former Dean. R. R. encouragements and good wishes.Acknowledgement I express my deep sense of gratitude. Director. S. humble and reverential gratitude to Dr.L.K.N. Jt. University. N.S. former Head. I profoundly thanks to Shri P. Department of Physics and former Heads Prof. Group Director and Dr.

Dr. Encouragements of Manak.J. Aditya. Sharma. Monu. Raj Kumar. Dr. Shri Sukha Ram. Anand.D. Sailendra. Sailesh.R.K. S. Abhisekh and all other friends are gratefully acknowledged. I also owe to thank to Ashok Soni. Avdesh. Amit Dave. Desh Raj. Manzoor. who added a new dimension of joyfulness during concluding period of this work. Uma Shanker Mirdha and Mrs. Dr.K. Mr. Rajvanshi. I appreciate the help of Mr. Chhagan. Neeraj and all scholars of Physics Department for all their encouragement. Grateful thanks are also due to Dr. Jt. Mr. Mr.K. Sharma. Thanks are also due to many others whose names the paper cannot accommodate but who lives in my memory never to be forgotten. S. Dr. Dr. Shri Hanuman Singh. Rashi Mathur. Patel and all professors of the department for valuable technical discussions. S. Sengwa.R. K. Ms. In the last but not the least. D. Thanks are also due to my sister Gayatri for endeavoring help. Vijay Singh.C. Affection for my little son Tanish. R. Dr. J. Sidharth. S. Naveen. Dinesh Kabra and Jagdish in the literature collection. G. I offer my sincere thanks to my wife Sarita for her endurance and patience during the course of this work. My special thanks go to colleagues Mr. Thanks are also due to Dr. Sharma. consistent encouragements and help in computer programming. (Jasa Ram) . Defence Lab for his kind cooperation and suggestions.work. I desire to express grateful thanks to Dr. Vadera. Director. Suresh. K. Manoj Patra. Negi. Manish. Manu Smrity for valuable suggestions. Dr. Sharma. Shri Babu Lal for all their encouragements. Dr.

…………………………………….5 : : : 12 17 20 ... ACKNOWLEDGEMENT……………………………....3 1. CERTIFICATE.2 : : An Overview Mechanism of electron transport between QWs and eigenstates of ADQW system QD as a tunnel device for coherent transport of electrons Role of nonradiative recombinations in nanosized semiconductors Outline of the present work 1 1 4 1..ϋ TABLE OF CONTENTS TITLE PAGE……. DEDICATION.………………………………………. TABLE OF CONTENTS……………………………… LIST OF PUBLICATIONS…………………………… ABBREVIATIONS AND SYMBOLS………………… i ii iii iϋ ϋ ϋi ϋii Chapter 1 INTRODUCTION 1.……………………………………….4 1..1 1.

1 2.ϋ Chapter 2 ANALYTICAL AND 2.2 : : PERTURBATION COUPLING Introduction Determination of zero perturbation position 44 44 45 .1 3.3 : : : THEIR Introduction Transcendental Equation for ADQW System Applications to Semiconductor Heterostructures (GaAs / AlXGa1-XAs) Transport optimization using variation in QW width Transport optimization using variation in confining potential Transport optimization using variation in material composition 23 EXPRESSIONS APPLICATION FOR TO 23 25 31 34 36 39 ASYMMETRIC DOUBLE QUANTUM WELLS SEMICONDUCTOR HETEROSTRUCTURES 2.2 2.3.3 : 2.2 : 2.1 : 2.4 : Conclusions 41 Chapter 3 ON THE POSSIBILITY WITH ZERO OF DESIGNING INTERACTING SEMICONDUCTOR QUANTUM WELLS 3.3.3.

1 5.1 4.ϋ 3.2 : : Introduction Transmission coefficient in terms of coupling coefficients QUANTUM FOR WELL AND PHASE EXPLANATION UNIVERSAL 71 71 78 .5 : : : Universality of zero perturbation position Coupling at zero perturbation Conclusions 49 51 53 Chapter 4 SINGLE 4.3 3.3 : : : ELECTRON Introduction Mechanism of charge transfer between QWs Conclusions CHARGING OF QUANTUM WELLS AND QUANTUM DOTS 55 55 59 69 Chapter 5 ELECTRON TRANSPORT THROUGH DOUBLE BARRIER BEHAVIOR 5.4 3.2 4.

2 : : RECOMBINATIONS IN NANO-SIZED SEMICONDUCTORS Introduction Calculation of Surface recombination velocity Semi-infinite Geometry Semi-conductor Slab of finite Thickness Cylindrical grain 91 91 92 95 96 103 6.3 : Separation of coherent and sequential tunneling coefficients and explanation of universal phase behavior in coherent transport Conclusions 82 5.2.2.ϋ 5.3 : Discussion & Conclusions 105 110 Chapter 7 SUMMARY & CONCLUSIONS REFERENCES REPRINTS OF PUBLICATIONS 116 .4 : 89 Chapter 6 NONRADIATIVE 6.2 : 6.3 : 6.1 : 6.2.1 6.

Dhariwal and Jasa Ram. Dhariwal. “Mechanism of charge transport across single electron states of coupled quantum wells and quantum dots”.ϋi LIST OF PUBLICATIONS 1. S.R.R. Jasa Ram and S. 69-75 (2005) . Dhariwal and Jasa Ram. S. communicated 4. S. in press (2006) 2. “Analytical expressions for asymmetric double quantum wells and their application to semiconductor heterostructures”. Physica B 363.R. Mag. Phil. Dhariwal and Jasa Ram. S. “Universal phase evolution in coherent transport of electrons through a quantum dot” communicated 5. Dhariwal and Jasa Ram. communicated 3. “On the possibility of designing interacting semiconductor quantum wells with zero perturbation coupling”.R.R. “Suppression of nonradiative recombination in small size semiconductors”.

q b. α2 E p.ϋii ABBREVIATIONS AND SYMBOLS QWs QDs QPC ADQW SDQW DQD QBS DBQW V1. a2 Quantum well(s) Quantum dot(s) Quantum point contact Asymmetric double quantum well Symmetric double quantum well Double quantum dot Quasi bound state Double barrier quantum well Confining potentials Quantum well widths Electron effective masses in quantum wells Electron effective mass in the barrier Wave vectors Attenuation constant in the barrier Energy eigenvalue Ratios of effective masses Barrier width . k2 α. a1. L2 m. α1. L1. m2 mb k1. m1. V2 L.

T2 τ tC tS SR fa β Fractional occupancies in the quantum wells Transmission coefficient Fermi Energy Width of resonance Gate potential Quantum well coupling matrix Inverse quantum well coupling matrix Barrier transmission matrices Decay time for quasi bound state Coherent tunneling coefficient Sequential tunneling coefficient Surface recombination velocity Sticking probability Cluster size parameter . ξ4 t Ef Γ U C Q T1.ϋii ξ2.

The recent interest in electron transport between QWs [2-8] and consequences of coupling upon eigenstates of coupled QWs [9-12] vis-à-vis charging of individual QWs [2.1 An Overview Confinement of electrons in nanosized structures known as quantum confinement has revolutionized the science in many streams [1]. the basic unit is a quantum well (QW). anomalous transport properties. 5. of which. qubits used in quantum . increase in optical efficiency. most noteworthy are enhancement of band gap. varied dielectric properties etc. For investigation of quantum confinement associated effects. 6. many new phenomena seem to emerge at this scale.Chapter 1 Introduction 1. In semiconductors. 18-24]. Such approach will also form the basis of understanding the mechanism responsible for a large number of applications of tunnel coupling of QWs like those in intersubband lasers [11. 13-17] have put on demand the necessity of quantitative understanding of such systems.

20. 56. Furthermore. particularly when studied vis-à-vis localization and delocalization of eigenstates in the individual QWs facilitated by means of parameters like external electric field. Simplest of the interacting QWs is an asymmetric double quantum well (ADQW) system. tetra hertz emission and absorption devices [28-32] etc. tuning QW sizes or varying material composition signifies major practical interests [3. particularly the recent reports of anomalous universal phase evolution [37-39]. study of artificial molecules [26. the behavior of eigenstates in coupled QWs plays crucial role in designing of quantum point contact (QPC) [33] for transport of electron through a quantum dot (QD) [34]. the variation -2- . memories [25]. The disordered structural features on such a small scale.Chapter 1: Introduction computations [2. 57]. wherein the light of practical use has become a reality even from silicon [49]. In addition to quantum confinement. particularly in case of etching produced porous silicon [50-54] requires a better understanding of the role played by nonradiative recombinations in enhancing optical efficiency [55]. 27]. this may help in understanding the fundamentals of coherent transport of electron through a QD [35. 36]. 8]. the recombination mechanisms have been a subject of wide investigation in accounting for the enhanced optical efficiency in nanosized structures [40-48]. The behavior of eigenstates of this system. Furthermore. Also.

6. 64]. the role of quasi bound states of the QD is crucial [62. 33]. 38] is not fully understood and remains a challenging problem [35. specifically at and around crossover are the studies of profound significance [2. From basic scientific point of view. 48]. Another important area of interest is electronics of quantum dots (QDs). 13-17]. Besides. in these systems as one tries to study the transport of electrons. 37]. 5. Based on quantum confinement related effects radiative recombinations -3- . QDs. 63]. The understanding of coherent transport through QDs will help in exploiting the wave nature of electron in highly miniaturized futuristic nano-sized electronic devices. 18-24. it is a fascinating problem to study [58-61]. nanosized QWs find important applications in optoelectronic devices [49. the interplay of eigenstates of ADQW system and the charge transfer between QWs. 11. evolution of phase of electron transmitted through the QD [37. In addition. 28. In particular.Chapter 1: Introduction of these parameters so as to bring the coupled system either at the crossover or at zero perturbation position depending upon the specific practical requirement forms the basis of various applications of coupled QWs [2-6. Efficiency of these devices depends on the relative magnitudes of radiative and nonradiative recombination rates [43. A QD can act as an artificial tunnel which is neither open nor closed and therefore.

However. little attention has been paid to the study of reduced size on the nonradiative recombinations [40. In the present study. Though. 70]. we shall like to understand the size dependence of nonradiative recombinations and its effect on the efficiency of opto-electronic devices.2 Mechanism of electron transport between QWs and eigenstates of ADQW system Determination of eigenstates of ADQW system has been a subject of profound interest. Worth mentioning is the perspective of ‘Man Made Quantum Wells’ by Kolbas and Holonyak [10].Chapter 1: Introduction have been investigated in much detail [65-69]. 1. However. This leaves a lot of scope to work on the understanding of the sciences of transport and recombination in this new class of materials and structures which the present thesis aims to present. These authors have used -4- . unabated the pace of miniaturization has made the quantum properties of electrons crucial in determining the design of the electronic devices. new and interesting problems are being posed by researchers. In the recent past. quantum properties of electrons will become indispensable when electronics based on individual molecules and single-electron effects will put back the conventional circuits.

In the envelop function method. 72]. 74]. variation of effective masses is used to take properties of the host into account. Numerical solution of Schrödinger’s equation has been used by Mourokh et al [3] to explain the effect of electric field on eigenstates of the double quantum dot (DQD) system. Similar numerical -5- . 71. transition between bonding (covalent) and anti bonding (ionic) behavior of eigenstates has been deduced. pseudo potentials. tight binding and at least in principle do not require the knowledge of the band offsets [17. As far as electronic states in heterostructures are concerned. the envelop function method focuses its attention on the modulation of the carrier wave functions which is due to the heterostructures itself [73.Chapter 1: Introduction computer simulation to illustrate interaction between coupled QWs and compared the results with those obtained by using Kronig-Penney model. Also.1. Microscopic calculations for the complete wave functions include one electron calculations. The band offsets should be the inputs to this approach. Theoretical developments in the tunnel coupling of QWs have been reviewed by Ferreira and Bastard [9]. These authors found a minimum separation in the energy eigenvalues of the adjacent states upon varying the electric field as shown the figure 1. theoretical developments from first principle calculations to effective mass approaches have been reviewed by Smith and Mailhiot [71]. On the other hand.

For smaller thickness of the intermediate barrier layer.1 Dependence of energy level separation on the applied dot to dot electric field [3] generalization of the Kolbas-Holonyak method [10]. This approach is. a multiple QW system becomes a supperlattice. -6- .1.Chapter 1: Introduction approach has been used by Neogi et al [11] to explain the intersubband transitions in coupled DQD system. Such systems have been dealt by solving Schrödinger’s equation for a periodic structure by Erman et al [12]. Numerical method of calculation of eigenvalues and eigenfunctions for doped intermediate barrier [75] and for symmetric double quantum well potential enclosed within two infinite walls [76] has also been reported recently. in fact. a Fig.

2 whereas figure 1. Hatano et al [2] have measured interdot tunnel coupling and showed that inherent asymmetry of the capacitances of the component dots allows the determination of the dot through which electron has passed. In fact the coupling between the QDs strongly influences the transport through the DQD system [5. Non invasive techniques have been employed to reveal the evidence of electron moving between the dots [7]. transport through QD requires it to be connected by QPC and engineering of QPC for optimum transfer have been analyzed by Zhang et al [33]. In practical cases of interest. In a novel experiment on interacting QDs. The QPC as charge detector has been used by Petta et al [5] to measure the microwave driven change in occupancy of -7- . The dynamics of the electron transfer between two QWs has also been studied by spatially transferring electron from one quantum well to its hole filled neighbour and detecting the near infra-red recombination luminescence [77]. Changes in the magnetization of DQD have also been used to investigate the crossings and anti crossings in its energy spectrum [78].Chapter 1: Introduction The eigenstates of ADQW system constitute the basis of the mechanism of electron transfer between QWs and is a subject of great practical interest. Schematic of the single anti crossing reported by the authors is shown in the figure 1. 33.3 shows the electric field induced symmetry of probability density in asymmetric system. 79-81].

1.1.3 Dependence of fractional occupancy of single electron η on the potential difference ∆ across coupled QDs [2] -8- .2 Schematic of single electron delocalized across both the QDs [2] Fig.Chapter 1: Introduction Fig.

depending upon the strength of inter-dot coupling. The coupling between QDs leads to bonding and anti bonding states whose energy -9- . Also.Chapter 1: Introduction charge states and study the manipulation of single charge in DQD. The understanding of DQD system finds direct applications in the study of bonds in artificial molecules [26] and forms the basis of molecular electronics. In the first case the electrons are localized on the individual dots while in the second case electrons are delocalized over both the dots. it has potential applications in microwave spectroscopy [27]. In these applications. As far as mechanism of electron transfer in double dot system is concerned. This inelastic tunneling with discrete energy exchange is known as photon assisted tunneling and has been extensively investigated [8. a time varying potential of microwave can induce inelastic tunnel events when electrons exchange photons of energy hν with oscillating field. current through the dot is resonantly enhanced only when two levels in the dots 1 and 2 align as shown in figure 1. the two dots form ionic like or covalent like bonds [3]. In weakly coupled QDs.4. 83-85]. the reference should be made to report by van der Vaart et al [82] which shows that when elastic tunneling process are the dominant transport mechanism. Charge delocalization in a tunable DQD has also been studied by DiCarlo et al [6] as a function of temperature and strength of coupling.

10 - .1.1.Chapter 1: Introduction Fig.4 Schematic potential landscape of the double quantum dot depicting the conventional understanding of electron transport between the QDs [82] Fig.5 Schematic pumping configuration for bonding state ψB and anti-bonding state ψA in photon assisted tunneling (PAT) [4] .

efficiency [28]. feedback effects [30]. The inset shows the positions of three lowest subbands (in meV) as a function of the narrow well width a1(in nm) for fixed values a2 = 2 nm and a3 = 10 nm [20] fascinating application area of these systems. Inter-sub-band lasers are another Fig. spectral line shape . The advantage of the pumping configuration is that these processes can lower the amount of current but they do not smear out the resonances [4].5. transport processes [19]. The DQD system has been studied for intersubband laser right from inversion of population [20].1.Chapter 1: Introduction difference is proportional to the tunneling strength between the dots.6 Schematic of inter-well transition in inter-sub-band laser. the pumping configuration is shown in figure 1. broadband wavelength operation [32]. For microwave spectroscopy of the strongly coupled double dot. temporal evolution [86].11 - .

As in an atom. for the first time. Yacoby et al [39] demonstrated in 1995 the measurements of magnitude and phase of the transmission coefficient through a quantum dot and proved directly. optical properties [89] to optical gain optimization [18].Chapter 1: Introduction [87]. negative differential conductance [94] etc. a single electron can tunnel through QD resulting in coherent transport. are other potential areas of the applications in nano-devices. Schematic of the prevailing understanding of electron transport in intersubband lasers achieved by optimization of thickness of the coupled QWs so as to arrive at crossover is shown in figure 1. In a novel ingenious interference experiment in semiconductors. the energy levels in a quantum dot become quantized due to confinement of electrons allowing formation of quasi bound states.6. relaxation kinetics [88].3 QD as a tunnel device for coherent transport of electrons Quantum dots exemplify an important trend in condensed-matter physics in which researchers study man-made objects rather than real atoms or nuclei [58. spin qubit [91].12 - . 61]. 31. that transport through the dot has a coherent . 1. In addition. 90]. At the same time. mid to far infra-red absorption [29. detector of high frequency quantum noise [92-93].

Since number and phase are conjugate variables. The field expanded substantially in 1998. Controlled decoherence was achieved [95-96] in a device with a quantum dot that was capacitevly coupled to a quantum point contact in close vicinity. the restoration of phase coherence has also been investigated [97]. The transmission phase displayed a number of unexpected properties. an improved four terminal device version of the experiment by Schuster et al [38] allowed to measure the phase of the transmission amplitude through the quantum dot.13 - . virtually the same transmission phase was found for a whole sequence of conductance peaks and in the conductance valley the phase displayed a sharp phase slip as shown in figure 1. the measurement caused the dephasing (decoherence) of electron states in the quantum dot. Their device consists of a GaAs/AlGaAs quantum dot with two adjustable quantum point contacts placed inside an Aharonov-Bohm (AB) ring which forms two arms of an electron interferometer.7. Most notably. The quantum point contact acted as a measuring apparatus for the number of electrons on the quantum dot. when it was realized that the coherence of quantum dot states can be controlled by external means. The measurement of phase and magnitude of the reflection coefficient of a quantum dot [98] have made further advancement in understanding of the coherence in QDs in terms of .Chapter 1: Introduction component. Further. In a step beyond the demonstration of coherence.

Chapter 1: Introduction

scattering. Recently, the interference experiments have been reported in mesoscopic systems [37] which shows that the phase behavior depends upon the electron occupancy of the QD. The explanations for the universal phase evolution in the transport through a QD, particularly, the phase slip at conductance minimum have been reviewed in 2000 by Gregor Hackenbroich [35]. Recently, M. Avinun-Kalish et al [37] also discussed the available explanations along with their shortcomings in explaining the experimental results. These authors have grouped the explanations in three main classes. The first group questions whether the measured phase is the ‘intrinsic transmission phase’ of the quantum dot or a modified phase due to multiple paths traversing the interferometer [99, 100]. The second, considers transport that is mediated by interplay of more than one quantum state. A common scenario assumes an existence of a dominant level strongly coupled to the leads, responsible for shuttling the electrons [101, 102]. After occupation the electron is unloaded to a localized level, weakly coupled to the leads, allowing the dominant level to be free again to transfer another electron. Hence, the observed phase is only that of the dominant level. Based on this idea other models examined only two levels, with one of the levels dominant, adding spins, adding interactions, or assuming a finite

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Chapter 1: Introduction

Fig.1.7 The universal phase evolution and phase slip in the conductance valley in electron transport through a QD [38]

temperature [103, 104]. Interaction between two levels was invoked also in a quantum dot where the plunger gate couples with different strengths to different energy states, leading thus to avoided level crossing and charge shuttling between levels [35]. The third class deals with specific energies where both the imaginary and the real parts of the transmission coefficient

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Chapter 1: Introduction

vanish [105]. These singular points, which explain the phase slips in the valleys, might result from a deviation from a strictly zero-dimensional system [35] or from the existence of Fano resonances in the dot [106]; but they can not explain the ‘in phase’ behaviour of all peaks. Naturally, one would expect the breakdown of every model for some tuning parameters, which we, thus far, have never observed. Still, some models may predict an ‘in phase’ behaviour for a very large sequence of peaks but not universal behavior. This necessitates the study of quasi bound states (QBS) of the quantum dot in the transport perspective. On the same line of thinking, Shao et al [59] has presented a numerical technique for open boundary quantum transmission problem which yields, as the direct solution of appropriate eigenvalues problem, the energies of (i) quasi bound states and transmission poles, (ii) transmission ones and (iii) transmission zeros. The influence of QBS on the carrier capture in the QDs has been investigated by Magnusdottir et al [107] and Ghatak et al [63] has calculated the mean life time of QBS of QW. The problem in the same point of view has also been dealt in terms of capacitance of the QD by Racec at al [108] and calculation for QBS in presence of electric field has been done by Ahn and Chuang [109]. Transmission coefficient from QBS perspective have also been

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The quantum confinement has redefined the research in luminescence wherein even silicon is considered as a promising lasing candidate for gaining light [49]. 111] in terms of quantum confinement. the study of luminescence in materials has been mainly confined around phosphors and the indirect band gap semiconductors materials like silicon were never considered appropriate candidates for luminescence applications.17 - . The easiest route to get light emitting silicon is by means of etching to produce porous silicon [50] which fetched much attention after the acceptable explanation of luminescence in porous silicon by Cullis and Canhan [64. Very simple explanations of the role of quantum confinement in silicon nanoclusters are .4 Role of nonradiative recombinations in nanosized semiconductors Until the advent of quantum confinement phenomenon. The quantum confinement effects have also been studied in amorphous silicon [112] as well as silicon nanoclusters produced by other methods [113]. 1.Chapter 1: Introduction calculated by Kim and Lee [62] and the same AB configuration has been calculated long back in 1984 by Gefen et al [110] but all these fails to provide satisfactory explanation of the universal phase behavior of transmission through a QD.

117]. Trwoga et al [118] has modeled the luminescent properties of the nanoclusters in terms of contribution of quantum confinement taking the example of silicon. 118].. The authors have studied the variation in oscillator strength and number of available free carriers with cluster size and size distribution.Chapter 1: Introduction available in literature [51. In fact. increase in oscillator strength [116] and lifetime [47. 119-122]. the quantum confinement has other consequences upon the luminescent properties viz. the increased efficiency is mainly attributed to enhanced radiative recombinations in the band tail states [44. it is the competition between radiative and nonradiative recombinations which determines the luminescence efficiency [43. Mehra et al [48] have also explained the luminescence . 66. 114]. Apart from band gap modulation. 51. 53. All such studies are aimed at the optical gain in nanosized structures [42. The study reveals that major contribution to luminescence is from radiative recombinations of confined excitons. John and Singh [43] have modeled the luminescent properties in terms of competition between an activated radiative process and a Berthelot type nonradiative process. 44. As far as recombination mechanisms in nanosized semiconductors are concerned.18 - . 45. 48]. A number of theories to explain the optical gap in silicon quantum dots have been reported [115].

However. to low dimensionality and to extremely low surface recombination rate. Vincignerra et al [41] have attributed enhanced luminescence efficiency in superlattices to the absence of relevant nonradiative decay processes as evident from the observed very long lifetime (about 0.3ms). 55. These authors have attributed high external photoluminescence efficiency to reduction in the nonradiative recombinations owing to low mobility. 41. Surface recombination velocity data also confirms the suppression of nonradiative recombination acting as enhancer of optical intensity [128]. little attention has been paid to . Role of nonradiative recombinations in studies pertaining to temperature dependence of luminescence has also been investigated [55.Chapter 1: Introduction data by considering competition between radiative and Berthelot type hoping process. Detailed studies of the radiative lifetime of porous silicon using photoluminescence decay measurements have been carried out by Hooft et al [40].19 - . There are a few reports which emphasises the role of nonradiative recombinations to explain the enhanced luminescence efficiency of nanosized semiconductor [40. 124. 123-127]. 125]. Neogi et al [123] have explained the enhanced efficiency in multi period QDs as compared to single period QD due to reduction in nonradiative processes.

details of which will be taken up in Chapter 4. In . of which applications to semiconductor heterostructures taking the example of GaAlAs / GaxAl1-xAs have been discussed considering the variation of QW width and confining potential. 1. In Chapter 2.Chapter 1: Introduction modeling of luminescence efficiency in terms of nonradiative recombinations to account for increased luminescence efficiency [129].20 - . The detailed analysis of the effect of coupling strength upon eigenstates of coupled QWs has been carried out in Chapter 3 using the analytical solution of the ADQW system presented in the Chapter 2. The variations of energy eigenvalues and eigenfunctions give an insight of the electron transfer in coupled QWs. Variation in the alloy composition has also been shown to produce effects similar to variation in QW width or depth. These analytical solutions find a large number of applications. analytical expressions have been derived for asymmetric double quantum well system for determination of eigenstates of coupled QWs.5 Outline of the present work The thesis is comprised of seven chapters including the present one. Outline of the work reported in the subsequent chapters is given below. Effect of coupling strength upon eigenstates has been presented.

21 - . The formulation clearly separates the direct and multiple reflection components in transport through a QD modeled as a double barrier quantum well and enable identification of . The analysis is used to explain the mechanism of electron transfer between coupled QWs. The explanation of the zero perturbation position has been given in terms of transmission line theory. transfer of electron between coupled QWs at zero perturbation position has been discussed in view of its possible applications. The analysis is based on the formulae derived in the Chapter 2. The sequence and significance of localization and delocalization positions of eigenstates in the two coupled QWs have been discussed and the effects of strength of coupling as well as asymmetry on these have also been presented. In Chapter 4. As an attempt to explain the universal phase evolution in coherent transport through a QD. a through study of mechanism of electron transfer between coupled QWs has been presented.Chapter 1: Introduction particular. this chapter is devoted to the study of zero perturbation position. The actual interplay of eigenstates of coupled QWs and charging of individual QWs has been presented. transmission coefficient has been derived in terms of QW coupling coefficients in the Chapter 5. Further. The universality of the zero perturbation position has been shown graphically as well as analytically.

These expressions have been used to study the nonradiative recombination rate as a function of size of confining structure and explain the enhanced optical efficiency in nanosized semiconductors in terms of suppression of nonradiative recombinations. In Chapter 6. The role of quasi bound states of QD in the coherent transport has also been brought into the formulation. . The summary of the work carrier out and gist of the conclusions drawn have been put together in the Chapter 7. thus providing an explanation of universal phase evolution.Chapter 1: Introduction coherent part of the transmission coefficient.22 - . the first principle semi-classical calculations have been done to derive expressions for surface recombination velocity for electrons confined between parallel plates resembling heterostructure and in cylindrical grain resembling quantum wire.

short wavelength light emission and absorption [28. semiconductor devices such as lasers [20]. 134]. 9.Chapter 2 Analytical expressions for asymmetric double quantum to wells and their application heterostructures semiconductor 2.1 Introduction Increasing demand of high density nano-sized quantum wells has resulted in extensive study of the mutual interaction of these systems. 8. single electron transistors [133]. quantum computation [2. 130-131]. dielectric and other material properties. optical. 132]. Such studies have great implications on the electronic. the problem finds direct applications in heterostructures. . Besides this. The simplest of these is an asymmetric double quantum well (ADQW) through which all basic features of interacting nanostructures can be easily understood [4.

24 - . 74] which allows calculation of eigenstates and eigen . most widely used of these being the Bastard’s envelop function method [73. However. Such numerical methods have been adopted by many worker [3. once an asymmetry is introduced either in terms of well width or depth such an inversion plane disappears and simple explanation in terms of symmetric and anti-symmetric coupling is not applicable. Solution of Schrödinger’s equation for a symmetric double quantum well (SDQW) with infinite outer boundaries is a text book problem which shows that the energy states of the individual wells couple themselves in two different ways namely symmetric and anti-symmetric interactions resulting in a splitting of the eigenstates.. for which the wave functions extend in the forbidden regions outside the ADQW. Further complications are added when external boundaries of the wells are limited to the same height as of the barrier between the two wells (a case of great practical importance). The problem can be solved by a numerical iterative method as outlined by Kolbas and Holonyak [10].Chapter 2: Analytical expressions for ADQW and their application……. This requires solution of Schrödinger’s equations in five different regions which are to be matched at four interfaces. memories [25] etc and form a basis for the study of artificial molecules [26-27]. 11]. The problem is solved in terms of an inversion plane at the center of the barrier around which a transition occurs.

1) is solved for ADQW system shown in the figure 2. We have solved analytically the Schrödinger’s equation for an asymmetric double quantum well (ADQW) system schematically shown in figure 2. the tight binding approximations and linear coupling of eigenstates have been used by many workers [71. 135-136]. function by iterative method by solving a set of equation at the boundaries. The solution finds direct applications in the design of electronic systems of practical interest.1 using the potentials and effective masses.1 which results in a much simplified mathematical formulation of the problem enabling a clear understanding of the underlying physics.Chapter 2: Analytical expressions for ADQW and their application……. Alternatively. such a method can be applied when barrier width is sufficiently large and interaction is weak. 2. h 2 d 2ψ ( x) + [E −V ( x)]ψ ( x) = 0 2m* dx 2 (2.25 - . However.. . A simple picture which appeals many is in considering two wells each having only one state and interaction between them is introduced as a perturbation [4]. validity of which is limited to weakly interacting systems [9].2 Transcendental Equation for ADQW System The time independent Schrödinger’s equation.

26 - . x→ V=0 -L1 Ψ1 Ψ2 0 Ψ3 b Ψ4 b + L2 Ψ5 V1 V= V1 V= V2 L1 b V2 L2 Figure 2.1 Schematic diagram of an asymmetric double quantum well system ..Chapter 2: Analytical expressions for ADQW and their application…….

− ∞ < x ≤ − L1 m1 .2) by matching the Ψ and (1/m*)dΨ/dx at boundaries as per Ben Daniel-Duke conditions [137].27 - . 0. − L1 ≤ x ≤ 0 mb . 1 ⎛ ∂ψ 1 ⎞ 1 ⎛ ∂ψ 2 ⎞ = ⎜ ⎜ ⎟ ⎟ mb ⎝ ∂x ⎠ x = − L1 m1 ⎝ ∂x ⎠ x= − L1 1 ⎛ ∂ψ 2 ⎞ 1 ⎛ ∂ψ 3 ⎞ = ⎟ ⎜ ⎜ ⎟ m1 ⎝ ∂x ⎠ x = 01 mb ⎝ ∂x ⎠ x= 01 1 ⎛ ∂ψ 3 ⎞ 1 ⎛ ∂ψ 4 ⎞ = ⎟ ⎜ ⎜ ⎟ mb ⎝ ∂x ⎠ x = a1 m2 ⎝ ∂x ⎠ x= a1 1 ⎛ ∂ψ 4 ⎞ 1 ⎛ ∂ψ 5 ⎞ = ⎜ ⎟ ⎜ ⎟ m2 ⎝ ∂x ⎠ x= L21 mb ⎝ ∂x ⎠ x= L21 (2.Chapter 2: Analytical expressions for ADQW and their application……. m2 . This determinant when equated to zero gives the allowed eigenstates. m =⎨ ⎪ ⎪ ⎪ ⎩ mb . mb . 0≤ x≤b b ≤ x ≤ L2 L2 ≤ x < ∞ (2.3) at x = -L1.. . ⎧ ⎪ ⎪ ⎪ V ( x) = ⎨ ⎪ ⎪ ⎪ ⎩ 0 V1 0 V2 0 ⎧ ⎪ ⎪ ⎪ * . b and b+L2 whereas the probability function is assumed to tend to zero at x→ ± ∞. These result in a set of eight equations for eight coefficients of integration. multipliers of which form a determinant.

e −αL αe 0 0 0 0 0 0 −αL1 sin k1 L1 − pk1 cos k1 L1 0 k1 0 0 0 0 − cos k1 L1 − pk1 sin k1 L1 1 0 0 0 0 0 0 0 −1 −α 0 0 −1 0 0 0 0 −αb 0 0 0 0 − cos k 2b qk 2 sin k 2b cos k 2 (b + L2 ) 0 0 0 0 0 0 =0 1 α −α e 0 0 e αb αe 0 0 αb e −αb − sin k 2b − qk 2 cos k 2b sin k 2 (b + L2 ) qk 2 cos k 2 (b + L2 ) − qk 2 sin k 2 (b + L2 ) − e−α (b+ L ) αe 2 −α ( b + L2 ) (2.4) .28 - ..Chapter 2: Analytical expressions for ADQW and their application…….

8) and the wave vectors k1 = 2 m1 ( E − V1 ) 2 m2 ( E − V2 ) . k2 = h h (2. Upon solving this 8x8 determinant. (α sin k1 L1 + p k1 cos k1 L1 ) X + (α cos k1 L1 − p k1 sin k1 L1 ) Y = 0 (2..5) with X = − α q k 2 (e + e + α 2 (e − e αb −α b αb −α b ) (−α cos k 2 L2 + q k 2 sin k 2 L2 ) ) (α sin k 2 L2 + q k 2 cos k 2 L2 ) . . V2 < E < 0 so that the attenuation coefficient (2.10) The corresponding wave functions are given by.9) are real.7) α= 2 mb | E | h (2. −α b Y = − pk1 qk 2 (e − e + α pk1 (e + e αb αb ) (−α cos k 2 L2 + qk 2 sin k 2 L2 ) −α b ) (α sin k 2 L2 + qk 2 cos k 2 L2 ) (2.6) Since we are interested in eigenstate of ADQW.29 - . In the above equations. m1 and m2 are effective masses of electrons in the two wells and mb is that in the barrier regions and their ratios are denoted by. we limit our solutions to V1 .Chapter 2: Analytical expressions for ADQW and their application……. p= mb m1 and q= mb m2 (2. we get a transcendental equation.

For -∞ < x ≤ -L1: ψ 1m ( x) = K eα x ..13) for b ≤ x ≤ L2: ψ 4 m ( x) = K 1 2α pk1 qk 2 sin 2k 2 b ⎡ ⎧ −α ( L1 +b ) (α − qk ) (α 2 + p 2 k 2 ) sin k L ⎤ ⎫ 2 1 1 1 ⎢ ⎪e ⎥ ⎪ ⎪ ⎪ 2 2 2 sin k 2 x ⎥ ⎢ ⎨ α ( L1 −b ) ⎧(α − p k1 ) sin k1 L1 + ⎫ ⎬ (α + qk 2 ) ⎨ ⎢ ⎪ +e ⎥ ⎬⎪ ⎢⎪ ⎥ ⎩2α pk1 cos k1 L1 ⎭⎪ ⎩ ⎭ Χ ⎢ ⎥. ⎩(α sin k1 L1 + pk1 cos k1 L1 ) cos k1 x ⎭ (2.Chapter 2: Analytical expressions for ADQW and their application…….30 - . for –L1 ≤ x ≤ 0: (2.14) . ⎥ ⎥ ⎦ (2. ⎫ ⎧ e−α ( L1 +b ) (α + qk 2 ) (α 2 + p 2 k12 ) sin k1 L1 ⎢ ⎥ ⎪ ⎪ ⎪ ⎢− ⎪ ⎥ 2 2 2 ⎢ ⎨ + α ( L1 −b ) (α − qk ) ⎧(α − p k1 ) sin k1 L1 + ⎫ ⎬ cos k 2 x ⎥ ⎬⎪ 2 ⎨ ⎢ ⎪ e ⎥ 2α pk1 cos k1 L1 ⎪ ⎩ ⎭⎪ ⎭ ⎣ ⎩ ⎦ { } { } (2.12) for 0 ≤ x ≤ b: ⎡ eα x (α 2 − p 2 k12 ) sin k1 L1 + 2 α pk1 cos k1 L1 ⎢ ψ 3m ( x ) = K 2 α pk1 ⎢+ −α x (α 2 + p 2 k 2 ) sin k L 1 1 1 ⎣ e e −α L1 { { } }⎤ .11) ψ 2m ( x) = K e −α L1 pk1 ⎧(α cos k1 L1 − pk1 sin k1 L1 ) sin k1 x + ⎫ ⎨ ⎬.

and for L2 ≤ x < ∞: ψ 5m ( x) = ψ 4 m (b + L2 ) e −α ( x − b − L2 ) (2. This essentially assumes that E-k relations are parabolic. shallow quantum wells with one or two energy states in each well are of great practical interest [5. Further. the effective masses will correspond to free electron mass and then p = q = 1.3 Applications to Semiconductor Heterostructures (GaAs / AlXGa1-XAs) In the transcendental equation (2. 81].Chapter 2: Analytical expressions for ADQW and their application…….15) The constant K in the above equations is determined by normalization of the wave function for the entire space extending from -∞ to ∞. we have taken constant effective masses for various regions. in the present day electronics a great interest has developed in potential wells formed in multi-layered semiconductor heterostructures.31 - .5). We choose here one of these systems as an example of application of the above equations.. 2. Non-parabolicity of E-k relations will involve nonlinearities and . When the potential barriers are formed in vacuum. The above equations are most general ones and may be applied to any type of ADQW system. We confine ourselves mainly to the study of these systems. though the conclusions are of general nature and can easily be extended to deeper wells with multiple states. However.

3Ga0.45 .083 X ⎧1. the probability distribution is equal in both the quantum wells and a complete delocalization exists whatever be the .0nm and X = 0. 0. A large number of reports are available on effective mass and conduction band offset variations with respect to composition parameter X [56. For such cases. The basic difference between SDQW and ADQW is that the asymmetry results in localization in ADQW. We have taken the following dependences from ref [140]. 0 ≤ X ≤ 0.45 < X ≤ 1. For SDQW. In actual semiconductors.0 (2. exact solution of Schrödinger’s equation is not possible. approximation methods are being used [138139] and may be helpful in getting exact characteristics of the material.. 140-143].7As) are plotted in figure 2. for simplicity of arguments. However. we have considered GaAs / AlXGa1-XAs heterostructure.0nm.32 - .3 (GaAs / Al0. the scope of the present paper has been limited to assuming effective masses to be energy independent. m* = 0.Chapter 2: Analytical expressions for ADQW and their application……. Using these parameters.1 X ∆Ec ( X ) = ⎨ ⎩0. the probability density and energy eigenstates for ADQW structure with L1= 2.14 X .067 + 0. As an illustration.2 at different values of barrier width b. non-parabolicities may exist which will then make m* a function of E.43 + 0.16) The effective mass given above is conductivity effective mass. L2= 4.

0nm at different well separations: (a) 5nm. .33 - .7As asymmetric double quantum well (ADQW) of QW widths L1= 2. Figure 2.Chapter 2: Analytical expressions for ADQW and their application…….3Ga0.5nm and in (d) energies of eigenstates are plotted against barrier width b.2 Probability density in GaAs / Al0. (c) 0.. (b) 1.5nm.0nm and L2= 4.

34 - .3. charge distributions remain largely localized in individual wells.3. the depopulated subband is aligned with the higher subband of the wider QW of appropriate size so that maximum transfer of electrons between the two becomes possible.. Next. 2.1 Transport optimization using variation in QW width Interwell transition in ADQW heterostructure comprising of one narrow and one wide coupled QWs is being used to get lasing via intersubband inverse population [20]. When the barrier width is reduced.Chapter 2: Analytical expressions for ADQW and their application……. It is a general belief that quick transfer of electron in . we apply these analytical formulae to some cases of practical interest. Contrary to this. strength of coupling. mathematical formulae presented here are much simpler and easy to use. the very fact of introduction of asymmetry attaches belonging of eigenstates to individual wells and for larger separations. In these systems. The electron energy eigenstates obtained here by using analytical formula are similar in nature to those obtained by Ferreira and Bastard [9] using numerical methods. Such an alignment requires determination of exact well width of wider QW for a given narrow QW such that difference of energy between eigenstates of the two isolated QWs is minimized. the probability distribution extends to the other well. The mechanism which works in the process is shown in figure 2. However.

0nm and b= 1.7As ADQW system. Figure 2.5nm have been used in fig (a) to (c) whereas dotted line in fig (d) shows an additional calculation for b= 1.3Ga0. L1= 4.Chapter 2: Analytical expressions for ADQW and their application…….0nm to depict the effect of increase in the strength of coupling.35 - . .3 Process of matched interwell transfer of electron by varying the width of larger QW coupled to a narrower one is shown for AlGaAs / Al0. Probability density of the matched state is shared equally between the two coupled QWs as shown in (b) and the corresponding energies are shown in (d) in which the inset gives the variation of difference of energy of the eigenstates ∆E= E2-E1 which shows a minimum at the same value of L2 for which probability of finding the electron in the two QWs is equal. In these calculations..

2. It is this equalization of probability that makes the transfer efficient under an elastic tunneling at the same energy rather than transfer of electron from one eigenstate to another. energy for photon or phonon assisted interwell transfer of electron can also be calculated using these analytical formulae. ∆E.2 Transport optimization using variation in confining potential The effect of variation of the confining potential by varying it for one of the wells while keeping the other as constant is shown in figure 2. The analytical formulae presented here can be used to calculate the exact width of the complementary QW which corresponds to minimum energy difference between nearest eigenstates in such a way that probability density of a particular eigenstate is shared equally between the two QWs as shown in fig. In addition.3.3(b).4 for a typically chosen GaAs / Al0.36 - . As one tries to minimize ∆E by changing width of the QW. the system under consideration is because of minimization of energy difference so that the two QWs resonate.0nm and .. the probability of finding the electron in each QW become nearly equal.3Ga0.7As ADQW with QW sizes L1= 2. one shifts the system slowly from an asymmetric to a symmetric one in which for the eigenstate under consideration. higher is the energy difference. 2. What we find here is that for a finite coupling of QWs there always exists a finite energy difference between eigenstates.Chapter 2: Analytical expressions for ADQW and their application……. Stronger is the coupling.

.3Ga0. L1= 4. Figure 2.5nm have been used in fig (a) to (c) whereas dotted line in fig (d) shows an additional calculation for b= 1. Probability density of the matched state is shared equally between the two coupled QWs as shown in (b) and the corresponding energies are shown in (d) in which the inset gives the variation of difference of energy of the eigenstates ∆E= E2-E1 which shows a minimum at the same value of L2 for which probability of finding the electron in the two QWs is equal.35 - ..7As ADQW system.Chapter 2: Analytical expressions for ADQW and their application…….0nm and b= 1. In these calculations.0nm to depict the effect of increase in the strength of coupling.3 Process of matched interwell transfer of electron by varying the width of larger QW coupled to a narrower one is shown for AlGaAs / Al0.

the electric field is equivalent to (V2-V1)/b in the present . The effect described above is similar to that obtained by applying an electric field. ADQW behaves like SDQW for this eigenstate.Chapter 2: Analytical expressions for ADQW and their application…….38 - . Here.0nm. This confirms the proposition that the size asymmetry can be neutralized by introducing confining potential asymmetry in an opposite direction. In the simplest term. 26]. The energy level separation at this point is similar to energy level splitting in SDQW. L2= 4.. As far as probability distribution is concerned. we find that by varying confining potentials V2 (or V1) the charge can be redistributed as shown in figure 2.4(b). Further. A large number of evidences exists in the literature that the asymmetry of size of ADQW can be neutralized by applying an external electric field [3. we note that the separation between the two eigenstates increases as one move away from the matched condition. since the purpose of electric field is also to create a potential difference between the two wells. We note that the ground state of narrower QW reaches a minimum energy difference with respect to second eigenstate of the wider QW at V2 ≈ 725meV making the behavior of ADQW system resembling a SDQW. The effect of change in V2 with respect to V1 as a matter of fact is equivalent to applying an electric field. we note that size asymmetry in ADQW results in the preferential distribution of charge in the individual wells to which the particular states belong.

3. we have plotted energy eigenstates and probability functions for typically chosen Al0.5(b) and (d) the size asymmetry can be compensated by varying the material mole fraction of the coupled QW. for eigenstate under consideration is equal. an effect similar to that obtained by varying QW width or confining potential.5.39 - . In addition.55As / AlAs / AlXGa1-XAs system with size parameters L1= 4. 2. Thus.. In figure 2.4(d) the separation of energy levels ∆E = E2-E1 against V2. our calculations provide an easy means of calculating the effect of electric field on the eigenstates of ADQW.Chapter 2: Analytical expressions for ADQW and their application……. formulations. we have plotted in the inset of figure 2.0nm and L2= 8. the estimation of Al mole fraction in the AlGaAs alloy itself is a very interesting problem and has been attempted . we find that minimization of energy difference ∆E as well as probability redistribution can also be accomplished by suitably selecting the alloy composition. Mourokh et al [3] by applying an electric field and at this point the probability of finding the electron in the two wells.3 Transport optimization using variation in material composition Results similar to those obtained by variation in V2 can also be obtained by variation in material composition of the alloy.45Ga0. Thus. As is clear from figure 2. To elaborate this point further.0nm. in which a minima is obtained similar to that reported by Lev G.

Chapter 2: Analytical expressions for ADQW and their application……..

Figure 2.4 Probability density in GaAs / Al0.3Ga0.7As ADQW of well widths L1= 2.0nm and L2= 4.0nm, QW separation b= 2.5nm and for confining potentials V1= 330meV and V2 equal to (a) 550meV, (b) 725meV and (c) 850meV are plotted. These show shift of charge density with variation of V2 and neutralization of size asymmetry for the given set of parameters for ground state at V2= 725meV. Variation of energy of the eigenstates with confining potential V2 is shown in (d) and inset shows the variation of difference of energy of the eigenstates of the two wells similar to that reported in the literature [11] for ADQW system by applying an external electric field. An additional dotted line in fig (d) shows calculation for b= 1.0nm to depict the effect of increase in the strength of coupling.

- 37 -

Chapter 2: Analytical expressions for ADQW and their application……..

rigorously by many researchers [56-57]. We here provide simple and easy to use analytical formulae for calculating Al mole fraction by measuring the band offset data of coupled heterostructure layer. In addition, certain properties of these heterostructures depends on the Al mole fraction [89] and mechanism underlying such effects can be better understood in terms of variation of energy states and probability redistribution in QWs using the analysis presented here.

2.4 Conclusions
In the present chapter, based on the first principles, we have derived analytical expressions for an asymmetric double quantum well system. This analytical approach provides the energy eigenvalues as roots of a simple transcendental equation and wave functions for corresponding eigenstates can be calculated using standard formulae provided by this method. In our calculation, we have provision to accommodate all necessary ADQW parameters such as individual quantum well widths and confining potentials, separation of wells, effective masses in different regions etc. Further, we have discussed some of the applications of the these analytical expressions for GaAs / AlXGa1-XAs semiconductor

heterostructures which reveal their simplicity in use and effectiveness in

- 41 -

Chapter 2: Analytical expressions for ADQW and their application……..

accommodating various material parameters as well as in understanding the underlying basic physics of ADQW. (i) Effect of variation of separation of the two wells upon the energy eigenvalues and corresponding wave functions has been studied for an ADQW having one eigenstate for each isolated well. The main feature of ADQW is localization of eigenstates in individual QWs as compared to SDQW in which a complete delocalization exists. In ADQW, delocalization of probability density increases as a result of coupling when the barrier width is reduced. Results thus obtained are in agreement with those reported in the literature using numerical methods. (ii) The effect of asymmetry can be minimized for a particular eigenstate by varying width of one of the QWs so that probability density in two coupled QWs becomes nearly equal for that energy level which in turn results in an efficient transfer of electrons. This occurs at the minimum energy difference between the eigenstate under consideration and its nearest state, corresponding to minimization of asymmetry and ADQW behaving like a SDQW for this state. (iii) The biasing of ADQW result in interesting properties and its variation can be used in tuning the QWs in a way similar to that obtained by

- 42 -

. investigating and optimization of properties of ADQW.43 - . (iv) The consequences of varying Al mole fraction on the properties of these heterostructures and estimation of Al mole fraction itself is of great practical interest and can be better understood in terms of band alignment and probability redistribution which in turn can be calculated using the analytical formulae presented here.Chapter 2: Analytical expressions for ADQW and their application……. Effects are similar to those obtained by applying an electric filed and are in agreement with those reported in literature. Thus a simple mathematical formulation provides an important method for understanding. varying QW width..

attempts have been made to couple the QW of the host material with another of larger width so that second eigenstate of the later coincides the ground state of the former to provide a means of depopulation [4. 11. While trying to understand these systems. For example in lasers. generally the interaction between the two QWs will perturb the original eigenstates [4]. we have come across an important property which shows that whenever a QW is coupled with another to form an asymmetric double quantum well system . However in doing so.1 Introduction A large number of efforts are being made to transmit electrons between quantum wells (QWs) elastically [3-6. 28]. 20. 20.Chapter 3 On the possibility of designing interacting semiconductor quantum wells with zero perturbation coupling 3. 28. 33].

(α sin θ1 + p k1 cos θ1 ) X + (α cos θ1 − p k1 sin θ1 ) Y = 0 with X = 2 α 2 qk 2 e αb 2 2 α (α 2 − q 2 k 2 )e − (α 2 + q 2 k 2 )e { cos θ 2 + αb −α b } sin θ 2 2 Y = 2α pk1 qk 2 e pk1 α − q 2 αb {( cosθ 2 + αb 2 2 k2 )e + (α 2 +q 2 2 k2 )e }sin θ −α b (3. 3. θ1 = k1L1 and θ2 = k2L2 shows that the eigenstates of this system obey the transcendental equation.Chapter 3: On the possibility ……quantum wells with zero perturbation coupling and if the phase traversed in the second QW is an integral multiple of π. Analytical expressions for eigenstates of this system have been discussed in Chapter 2. The results may find important applications in interacting heterostructures like those used in designing inter-sub-band lasers [18-24] and laterally coupled quantum dots (QDs) [2-3.45 - .1) .2 Determination of zero perturbation position The two coupled QWs of arbitrary size and depth form an asymmetric double quantum well (ADQW) system shown in the figure 2.1. This condition of zero perturbation coupling is universal and is independent of the strength of interaction. 33]. the eigenstate of the first QW remains unperturbed. which when expressed in terms of phase angles a free wave would travel in the two QWs.

we find that for every QW for a given energy level of interest. as is clear from the figure even for the best chosen width L2 around this point some energy gap always exists and a perfect elastic coupling is impossible to achieve. we limit our solutions to V1 .1) by keeping the host QW width L1 as constant and by varying the width L2 of the second QW for GaAs / Al0.7As ADQW system for various strengths of coupling. V2 < E < 0 . the later being determined by barrier width. On the other hand. b. at point ‘Q’ the energy eigen value of the coupled system is exactly equal to that of the host and the host finds continuity with the other QW without being perturbed at all. It is only at a triviality of infinite barrier width that the two eigenstates coincide. We have plotted in Fig.46 - . Attempts of tuning these QWs have mostly remained confined around points marked ‘P’ in the figure. However. When adjusting the QW width L2 a matching is said to have been achieve.3Ga0. Since we are interested in eigenstates of ADQW. . independent of the strength of coupling. 1.Chapter 3: On the possibility ……quantum wells with zero perturbation coupling where effective masses in the two QWs and the barrier are m1. q = mb / m2. the roots of equation (3. m2 and mb respectively and their ratios are represented by p = mb / m1 . there exists another well to which it can be coupled without perturbing the original eigenstate. so that the attenuation constant α in the barrier and wave vectors k1 and k2 in the two QWs are real. Thus.

where strength of coupling is varied by changing the barrier width b.1 Energy eigenstates of two coupled QWs forming asymmetric double quantum well system are plotted by keeping the width L1 of the first QW fixed and varying the width L2 of the second QW. mb = 0.7As system using m1 = m2 = 0.Chapter 3: On the possibility ……quantum wells with zero perturbation coupling Figure 3.3Ga0.067mo. The values are calculated by taking numerical example of GaAs / Al0.0919mo. L1 = 2.0nm and V1 = V2 = 330meV. .47 - . All eigenstates irrespective of the strength of coupling e-α b pass through a common point ‘Q’ which shows zero perturbation coupling at these points.

where strength of coupling is varied by changing the barrier width b. All eigenstates irrespective of the strength of coupling e-α b pass through a common point ‘Q’ which shows zero perturbation coupling at these points.0nm and V1 = 330meV. mb = 0.3Ga0.48 - .7As system using m1 = m2 = 0.067mo. The values are calculated by taking numerical example of GaAs / Al0. L1 = 2. .0919mo.Chapter 3: On the possibility ……quantum wells with zero perturbation coupling Figure 3.2 Energy eigenstates of two coupled QWs forming asymmetric double quantum well system are plotted by keeping the widths L1 and L2 of the QWs fixed and varying the potential V2 of the second QW.

the energy level E1 remains unchanged whereas the wave function extends to the other QW. in experimental conditions both L2 and V2 can be varied to achieve a fine tuning. a corresponding k2 can be calculated and L2 can then be determined to satisfy the above condition. we have plotted eigenstates as a function of phase angle φ2 = k2L2 in figure 3. .3 Universality of zero perturbation position Universality of this property of the point ‘Q’ in Fig. 3. for an eigenvalue E1 of the host QW. the equation becomes independent of the barrier width b and reduces to (α 2 − p 2 k12 ) sin θ1 + α pk1 cos θ1 = 0 (3. These two graphs clearly shows the universality of zero perturbation position at φ2 = k2L2 = nπ irrespective of the variation of k2 or L2. Further. For this value of L2 even after coupling the QWs.Chapter 3: On the possibility ……quantum wells with zero perturbation coupling Similar effects have been obtained when k2 is varied by varying V2 instead of L2 as shown in figure 3. 3. Thus. In order to make our result further explicit.2) Roots of this equation give eigenstates of isolated host QW of width L1.1 can be proved by using the analytical result given by equation (1).3(a) by varying L2 and in figure 3.2.49 - .3(b) by varying k2 (in terms of V2). By putting θ2 = k2L2 = nπ where n is an integer.

50 - .2 respectively.1 and 3.3 Graphical representation of zero perturbation position at φ = k2L2 = nπ obtained by (a) variation in L2 and (b) variation in V2 using the parameters used in figures 3. All states passes through φ2 = k2L2 = nπ. Energy eigenstates of two coupled QWs forming asymmetric double quantum well system are plotted as functions of φ2 = k2L2.Chapter 3: On the possibility ……quantum wells with zero perturbation coupling Figure 3. .

the solution ψ = K e −α x is a valid solution throughout the barrier.4 the wave functions ψ and find that the form of distribution function in the first QW remains invariant at all strengths of coupling. This shows that coupling with the second QW does not reflect the wave backward and a perfectly matched coupling can be achieved. ⎛α ⎞ dψ = −⎜ ⎟ ψ ⎜ p⎟ dx ⎝ ⎠ (3. if a barrier is introduced at this place. Since. it will always find continuity. introduction of barrier of any width at x = L1 leaves the eigenstate .5 and variations in the fractional occupancies in the two QWs as a function of barrier width in figure 3.4 Coupling at zero perturbation To further our understanding of the system around this point.3) If the ψ function of a large QW formed by combining widths L1+L2* where L2* is the width of the matched QW corresponding to the energy E1 the condition (3) can be found to exist at x = L1.51 - . The absence of reflection can be understood by noting that for an isolated QW a solution ψ = K e −α x exists in the barrier region and at the boundary of the QW we have. we have plotted in figure 3.Chapter 3: On the possibility ……quantum wells with zero perturbation coupling 3. This shows that in a QW of width L1+L2*. Whereas the probability density ψ*ψ in figure 3.6 show that its magnitude reduces as the strength of the coupling is increased.

(b) the probability densities Ψ* Ψ and (c) the fractional occupancies in the two QWs are plotted for coupled QW system with the host QW width of L1 = 2nm matched with a second QW of width L2 = 5. As the strength of the coupling is increased.3nm so that energy eigenvalue of the state remains constant at E = 127.52 - . .4 (a) The wave functions Ψ.Chapter 3: On the possibility ……quantum wells with zero perturbation coupling Figure 3.3 meV. the occupancy in the coupled QW increases without any change in the energy eigenvalue as well as the wave form of the host QW.

Thus. On the other hand. for every QW for a given eigenstate another QW can always be found which is completely matched with the host and electron can tunnel from the host to the guest without perturbing the former. when the phase elapsed in the second QW is an integer multiple of π.4 Conclusions For a given eigenstate of a quantum well (QW). The situation here resembles that of a transmission line terminated with characteristic impedance which acts effectively as an infinite line with no reflection and any half wavelength line added in between acts as 1:1 transformer. the condition at the two boundaries remains essentially unchanged because of symmetry (or anti-symmetry). This new type of coupling may find important applications in heterostructures in which the barrier width may vary because of disorders at the interfaces and in coupled quantum dots where separation . 3. it is always possible to find another QW in such a way that the coupling leaves the original eigenstate of the host QW unperturbed irrespective of the strength of interaction.53 - . The condition is universal and is met with whenever the second QW has appropriate width and depth so that phase traveled by an electron wave through it is an integral multiple of π.Chapter 3: On the possibility ……quantum wells with zero perturbation coupling unperturbed.

This may also find useful applications in heterostructures and quantum dots in which monochromaticity is an essential requirement. the matched coupling described above is applicable for multiple QWs where a host QW can be coupled to as many QWs as required and none of them will disturb the original eigenstate.54 - . .Chapter 3: On the possibility ……quantum wells with zero perturbation coupling between them may not be controllable to a fine precision. It may be further pointed out that though we have analyzed only a system of two QWs. An elastic coupling between QWs reduces the possibility of energy loss in electron transfer and may find important applications in nano-electronic devices.

Change in fractional occupancy as the coupled system is varied around energy crossovers has been presented by these authors. 13-17].1 Introduction The recent impetus in research pertaining to charging in coupled QWs and QDs from various aspects and in variety of systems has put forward the requirement of a detailed quantitative study of interplay between single electron charging and quantized energy states of the coupled system [3-6. the photon / phonon assisted tunneling based applications require a detailed understanding of mechanism of charging of . Furthermore. The novel application like spin entanglement using charging in DQD by Hatano et al [2] has increased the significance of such studies.Chapter 4 Single electron charging of quantum wells and quantum dots 4. These authors have presented charging diagram around the crossover position and explained the delocalization of states in terms of symmetry and asymmetry of coulomb diamonds.

The formation as well as control of covalent / ionic bonds in DQD system also requires the detailed understanding of charge transport. The system acts as if a bigger QD (QPC) is coupled with smaller one for transfer of charge and therefore. Even the manipulation of single charge in coupled QDs has been shown by Petta et al [5] using microwave excitation. such studies as well as the designing of QPC [33] have put on demand the understanding of charge transfer in QDs. The demand of quantitative description of charging of quantum structures is further enhanced by experimental studies for imaging of single electron charge states in QDs using various techniques [13.Chapter 4: Single electron charging of quantum wells and quantum dots QWs / QDs vis-à-vis energy eigenstates of the system. for the study of transport through a QD.56 - . In addition. it is required to be connected with some QPC. the explanation of anomalous universal phase evolution in electron transport through a QD by Hackbroich et al [60] in terms of avoided crossings can be better understood if charging and discharging profiles are studied around the crossovers. 144-147]. Moreover. These authors have accurately determined the inter dot coupling using the charge readout. These authors conclude that the understanding of charge manipulation across DQD is crucial for spin manipulation experiments and the same has been shown by Hatano et al [2]. It is . Di Carlo et al [6] has used QPC for charge readout to investigate charge delocalization.

Averin et al [14] accommodated the energy quantization in the formulations to explain the charging of QWs and QDs by taking into account the change in electrostatic energy of the capacitance of QWs and QDs.Chapter 4: Single electron charging of quantum wells and quantum dots to be noted that Silvestrov and Imry [101] have given an explanation of universal phase evolution using a model for charging of a QD. such an alignment of states is never achieved for . The authors have emphasized the importance of discreteness of the charge accumulated but have given only the extension of the conventional description [148] of the single electron charging effects. These authors have accounted for the symmetry properties of the resonantly coupled QD states to govern the charging of QD. In fact. In this analysis. Later. Fermi level of the emitter is supposed to align with discrete levels of the QD to resonantly transfer charge to it. The charge re-distribution in the tunneling process has been studied by Fong et al [149]. Though.57 - . The single electron charging effects in small area metal tunnel junctions have been reviewed by Averin and Likharev [148]. discreteness of charge accumulation in the QWs has been considered but actual interplay between single electron charging and eigenstates of the system is not obvious in the formulation. The analysis is based on the scaled version of density functional theory and has been presented in terms of bonding and anti-bonding molecular resonant tunneling states between coupled QDs.

The dispersion relations for ADQW system calculated using finite difference approximation along with eigen functions have been given by these authors to explain the reduction of tunneling time. the coupling itself greatly influences the charging characteristics. Moreover. The effect of strong shift in the QDs energy states upon addition of single electron has been considered by Johnson et al [16] to explain their experimental findings. These authors have analyzed the single electron charging in QDs in the transport experiments taking into consideration 0D states of QDs. a qualitative picture of charge transfer in terms of inter band . Although.58 - . These authors have observed reduction in tunneling time for fixed barrier width as the system is moved from minimum energy difference to be greater then LO phonon energy. All these investigations lead to a common theme of charging of QDs and QWs in exact quantization framework while taking into account the effect of finite coupling through which charge is actually transferred. An experimental study of tunneling time in GaAs / AlxGa1-xAs ADQW system has been presented by Roussignol et al [17]. An ADQW may form the most appropriate system to bring the interplay of actual quantization of energy states and charging effects in one frame work so as to resolve finer features of charging of QWs and QDs together with exact quantitative analysis of the mechanism of charge transport.Chapter 4: Single electron charging of quantum wells and quantum dots any finite coupling of emitter with QD.

the authors have concluded that charge transfer mechanism should not be sensitive to the effect of band banding. The simplest method for understanding the mechanism is to investigate the electron states of an ADQW system in which electron states can be manipulated by applying gate voltages.Chapter 4: Single electron charging of quantum wells and quantum dots relaxation has been discussed in this paper. Such a conclusion may be a result of the qualitative picture of charging. Thus. 4. asymmetric double quantum well (ADQW) system forms a basis for understanding the mechanism of electron transport between QWs and QDs. The conventional understanding of the charge transfer is that each QW has discrete energy states and as the potential energy of the QWs is varied. Also. Quantitative analysis presented in this chapter clearly brings out the finer details of charge transfer at the cross over and satisfactorily explain the recently reported experimental results of Hatano et al [2]. these quantum wells have asymmetry of size as well as potential energy of which the later can be varied by applying gate voltages.2 Mechanism of charge transfer between QWs A quantitative analysis of the transport of electron through coupled QWs is crucial in designing and implementation of nano electronic devices. In general.59 - . the states align . the laterally coupled QDs can be modeled as two QWs coupled through a barrier.

3Ga0. we have considered example of GaAs / Al0. where ξ1 = ∫ψ ψ 2 dx * 2 − L1 0 ∞ −∞1 ∫ψ ψdx * (4. in which we have also arrived at a similar conclusion. in which delocalization of energy states of the two QWs occurs one after the other separated by a potential energy gap. we find that the charge transport takes place in three steps. a closer look at the one electron states of the coupled system shows that the states never align but slip around the crossover positions as the QW depth is changed [4.4) and ξ 2 = ∫ψ ψ 4 dx * 4 0 L2 ∞ −∞1 ∫ψ ψdx * (4.5) For understanding the mechanism of charging of QWs and QDs.Chapter 4: Single electron charging of quantum wells and quantum dots themselves to allow a resonant tunneling [82]. we first calculate the fractional probabilities of electron occupancy in the two QWs defined by ξ1 and ξ2 respectively. the mechanism of electron transfer is delocalization of electron states around the crossover. In Chapter 2. When we go through further details of calculations.7As ADQW system. in which one QW is treated as host from which an electron is to be transferred to . For this. we have given an analytical solution for an ADQW system. As pointed out by Hatano et al [2]. 9] (here by changing the gate voltage). However.60 - .

we have plotted in figure 4. As k2 is increased. we here mean that the two isolated QWs will have energy eigenstates E10 and E20 which meet at a common point in the E-k2 plane. the first eigenstate is mostly localized in the first QW. . at the point A there is a delocalization in which probability of finding the electron in his state becomes equal in two QWs (ξ1 = ξ2). the states get almost completely localized in the second QW with next higher state E2 having same fractional occupancy also localized in the second QW.1(c).61 - .1(a). At the extreme left. Now. This minimum of ∆E is shown in figure 4. We start our argument with states around a single crossover. these states interact in such a way that energy states slip around this crossover and the crossover is avoided. The energy difference ∆E = E2–E1 goes through a minimum as one changes k2 (by changing the potential energy V2 of the second QW). these coupled energy states become E1 and E2 shown by solid lines in the figure. By crossover. It is around this minimum rather than exact crossover position that the entire charging process takes place. the fractional occupancies for the two states E1 and E2 as function of wave vector k2. This is shown in figure 4.1(b). at the point B. In order to understand charging process.Chapter 4: Single electron charging of quantum wells and quantum dots second QW to which a gate voltage is applied. As one tunes the system towards the ∆E minimum position. When coupled together.

Chapter 4: Single electron charging of quantum wells and quantum dots Figure 4. . Charging diagram clearly shows exact interplay between eigenstates of coupled QWs and their charging wherein point A corresponds to delocalization of state E1. electron remains in second QW between A and C and in first QW beyond this region of sharp transition. (b) Energy difference between the eigenstates of coupled QWs. Thus.62 - . (c) Fractional occupancy ξ1 in the first QW is shown by dashed lines whereas ξ2 in the second QW by solid lines. point B corresponds to localization of both states in the second QW signifying the actual charge transfer position and point C to delocalization of state E2 in k2-E space.7As system using typical ADQW parameters with L1 = 200nm and L2 = 50nm. Solid lines are for b = 5nm whereas dotted lines show the energy crossover.3Ga0.1 (a) Eigenstates of GaAs / Al0.

.2 Eigenstate changing its parity around the probability crossover position which signifies change of eigenstate.63 - .Chapter 4: Single electron charging of quantum wells and quantum dots Figure 4.

64 - . The energy states when plotted for repeated crossovers are shown in figure 4. a delocalization at point A. the state function ψ for level 1 up to the point B. a sharp localization in the second QW at point B and a delocalization of the next state at point C. Thus.Chapter 4: Single electron charging of quantum wells and quantum dots Beyond this point. Let us generalize the discussion by considering the interplay of eigenstate of the coupled system and charging of individual QWs. the state E2 is again localized in the first QW. Around this point B. Subsequent to this. takes place at the minimum energy separation between the interacting states. thus energy eigenstate of interest switches from E1 to E2 and the coupling is changed from symmetric to anti-symmetric as shown in the figure. we have plotted in figure 4. To elaborate this point further.2. This replacement of E1 by E2 by means of potential energy variation changes symmetry of the system and the coupling changes from symmetric to antisymmetric one or vise versa. E2 replaces E1 and the system is again delocalized at point C. in which each energy eigenstate show a staircase type of variations going . the entire process goes in three steps.3. Thus. where actual crossover of probability takes place and around which the mechanism of charge transfer actually occurs. Now. state E2 replaces E1 by the process of delocalization and re-localization in which a sharp localization in the second QW which is being tuned.

Chapter 4: Single electron charging of quantum wells and quantum dots Figure 4.3 Fractional probabilities of electron occupancy in the coupled QWs along two adjacent energy eigenstates in the energy spectrum of ADQW system showing the actual interplay of eigenstates of coupled QWs and charging of individual QWs. . Dashed lines have been used to show fractional occupancies in first QW whereas solid lines shows these in the second QW. Sharp rise in the fractional occupancy in the second QW around the crossover explains the mechanism of electron transfer in coupled QWs and QDs.65 - . Thicker lines correspond to state E1 and thinner to state E2.

Thus. This process continues for all the crossovers as shown in the figure. Thus. The occupation probability for electron eigenstate slips sharply from first QW to second QW resulting in a movement of energy eigenstates one step downward with higher state replacing the original state. . the process of charging of second QW is around the crossover. the states of the first QW get delocalized in the second QW sharply forcing the system to move one step down on the energy spectrum and localizing again in the first QW. this gives rise to periodicity in the eigenstates with energy discontinuity around the crossover position. say at the Fermi level of the system. Thus. occupancy in the first QW switches ‘ON’ to ‘OFF’ as one pass through crossover. We find that. we have plotted fractional occupancies ξ1 and ξ2 in the two QWs for two energy states E1 and E2. In other words. However. the entire set of energy levels goes down one step with higher energy state replacing the lower one. If seen at a particular energy. around the crossover. The thicker lines are for the state E1 whereas thinner ones for state E2. ξ2 rises sharply around the crossover and settling down to smaller value at off resonance. The dashed lines show fractional occupancy ξ1 for first QW whereas solid lines for ξ2 the fractional occupancy in the second QW.66 - . here our concern is mainly the charging process and therefore.Chapter 4: Single electron charging of quantum wells and quantum dots down by one step around the crossover.

3Ga0. Here. L2 = 50nm for b = 7nm.67 - . The actual electron transfer position is found to be at the minimum of energy difference between the two states irrespective of strength of coupling. difference in energy eigenvalues ∆E and fraction occupancies ξ1 and ξ2 in the two QW using the GaAs / Al0. However.7As ADQW with L1 = 200nm. decrease of b signifies the increased coupling strength.4 Effect of strength of coupling upon charging of coupled QWs is shown by plotting the energy eigenstates. the spread of delocalization ∆k as well as ∆E increases with increasing coupling strength.Chapter 4: Single electron charging of quantum wells and quantum dots Figure 4. . 5nm and 3nm.

68 - . However. difference in energy eigenvalues ∆E and fraction occupancies ξ1 and ξ2 in the two QW using the GaAs / Al0.7As ADQW with L2 = 200nm. the spread of delocalization ∆k increases with increasing asymmetry whereas a simple correlation may not exist for dependence of ∆E. 200nm and 225nm. The actual electron transfer position is found to be at the minimum of energy difference between the two states irrespective of asymmetry of coupled QWs.3Ga0. b = 5nm for L1 = 175nm.Chapter 4: Single electron charging of quantum wells and quantum dots Figure 4. .5 Effect of asymmetry of coupled QWs upon their charging is shown by plotting the energy eigenstates.

Similar types of effects are shown in figure 4. the conclusions can be directly applied to the coupled QDs also. The value of ∆E is itself is a function of coupling strength. This changes ∆k as well as ∆E but a simple correlation may not exist. 4. we change the barrier width b. However. essentially behave as a system of coupled QWs in the direction of coupling and therefore. in all cases.5 obtained by changing asymmetry by means of QW width L1 while second QW width L2 has been kept constant.Chapter 4: Single electron charging of quantum wells and quantum dots To study the effect of strength of coupling. QDs when coupled. We find that width of the transition region ∆k = kC–kA increases with increasing strength of coupling corresponding to lower value of width barrier b. we find that determination of fractional occupancy ξ1 and ξ2 of finding electron in the two QWs is crucial for understanding the mechanism of charge transfer between two QWs. Smaller values of b correspond to higher strength of coupling and hence result in higher ∆E also as shown in figure 4.6 Conclusions To conclude.69 - . the crossovers in the probability take place at the minimum of energy separation ∆E. We find that the energy separation between the two nearest energy states is minimum at the probability crossover position and around this .4.

In the first step. although a simple correlation may not exist in this case. Increasing strength of coupling by reducing barrier width b increases ∆E as well as ∆k. The process of charge transfer takes place in three steps. However.Chapter 4: Single electron charging of quantum wells and quantum dots point. Varying L1 (or L2) may also change ∆k and ∆E. the entire spectrum of energy eigenstate gives an appearance of staircase type of picture in which each state goes down by one step around the crossover at which the occupation probability sharply changes their belonging from first QW to second QW and then giving rise to a resonant effect. The process of electron transfer involves one energy state being replaced by another of opposite parity and coupling changes alternatively between symmetric and anti-symmetric one. This describes the interplay between energy eigenstates of coupled QWs and the charging of individual QWs. the eigenstates localized in the first QW delocalized which are then localized sharply in the second QW and then get delocalized again to get localized in the first QW once again. . each resonance corresponding to an electron transfer and the spectrum going down by one step.70 - . The width of the crossover is determined both by the strength of coupling and the asymmetry. the entire mechanism of electron transfer takes place. Next. the energy crossover position is not exactly coinciding with the probability crossover position in the E-k plane.

Chapter 5 Electron transport through double barrier quantum well and explanation for universal phase behavior 5. The most important of such a system is the study of transport through a QD. These bound states of coupled QWs are crucial for determination of charging in such system and what exactly required is the interplay of these two. For such studies. if we look at electron transport through an open system in which a free electron wave is transmitted through a closed system. Now. a QD is modeled as an artificial tunnel having two barriers coupled by a QW and free electron wave .1 Introduction In the previous chapter. the situation might be quite different. we have investigated the charge transfer in ADQW system which is basically a closed system and allows formation of bound states.

However. The study of QBS of the quantum dot in transport perspective has been attempted by many researchers. For infinite barriers.Chapter 5: Electron transport through DBQW & explanation of universal phase behavior transmission is studied through it. 150]. Time dependent studies reveals the life time of these QBS [62-63. the QD supports only the formation of bound states whereas for finite barriers. These authors have used numerical technique to evaluation energies of quasi bound states and transmission poles. long lived states referred to as quasi bound states (QBS) also exists. While investigating the interaction of carriers in QBS of QD. transmission ones and transmission zeros and as an example double barrier resonant tunneling has been investigated. a strong electron phonon coupling exits giving rise to another type of carrier capture. the role of these QBS and discrete QD states in spatial transfer of electron wave through this quasi bound region may be crucial in determining transport through the QD. Racec at al [108] have investigated QBS at a transition from nearly closed to open system and . the open boundary transmission problem has been reduced to eigenvalue problem by Shao et al [59]. Magnusdottir et al [107] have found that for a level separation between QBS and a discrete QD state in the vicinity of the phonon energy. By forcing the incoming source term to zero.72 - . The bound character of the region confined between tunneling barriers is determined by height and width of these barriers.

the formulation incorporates the transmission coefficient of DBQW but it does not involve parameters of energy discreteness explicitly.Chapter 5: Electron transport through DBQW & explanation of universal phase behavior found that these develops a separate type of resonance and its energy lies in classically allowed regime. evolving by π through . Exact calculation for energy level and resonant width of QBS in a QW with an applied electric field has been done by Ahn and Chuang [109] by solving the Schrödinger’s equation. These authors have found quantitative agreement of such transition in capacitance experiments on metal oxide semiconductor (MIS) type heterostructure. The authors have devised a method for determination of tunneling lifetime. Although.73 - . Ghatak et al [63] have given analytical expressions for the mean life time of the QBS of a single QW. So far as transmission through a double barrier quantum well (DBQW) is concerned. Their calculation gives both the resonance position E and width Γ for the complex eigenvalue E – iΓ/2 of the system. particularly in explanation of the recent reports of universal phase behavior [37-38]. The role of QBS and discrete states may be crucial in determining coherent transport through a QD. The phase of electron wave transmitted through a QD shows a universal behavior. Kim and Lee [62] have presented an analytic method for solving time dependent Schrödinger’s equation.

74 - . the phase returns sharply to its starting value. This coherent transmission is Figure 5.1.Chapter 5: Electron transport through DBQW & explanation of universal phase behavior each conductance peak and in the conductance valley. The transmission of electron through a QD . 37] which predict a phase change of π for each transmission cycle without a phase slip in between as shown in figures 1.1 Recently reported universal phase evolution and phase slip in the conductance valley for higher electron occupancy and anomalous behavior for lower occupancy in electron transport through a QD [37] directly in contradiction with existing theories [35.7 and 5.

Büttiker [151.75 - .B. Transmission probabilities have .1) where Ef is Fermi energy of electrons transmitted through the device and En and Γ the energy and width of resonance in QD. Schuster et al [38] have described the coherent part tQD of the transmission amplitude through the QD by the BreitWigner expression [152] tQD = C n iΓ 2 (E f − En )+ i Γ 2 (5.Chapter 5: Electron transport through DBQW & explanation of universal phase behavior modeled as a QW confined between two barriers has been thoroughly investigated in the literature [35. The formula for conductance by Gefen et al [110] G= 2e h 2 (De 2 (Ae 2 iϕ iϕ + Be − 2 iϕ − iϕ ) 2 + Ee +C ) (5.2) where φ is the dimensionless flux and constants A. 151] but no satisfactory explanation is available so far [37]. As far as transmission coefficient is concerned.. formulae have been given by Gefen et al [110]. directly gives coefficient as a function of magnetic flux enclosed by Aharonov-Bohm (AB) ring used in interference experiments and formulae are expressed in terms of transmittances of individual barriers but the role of sandwiched bound region is not obvious. 110. 153] and many other authors. These authors have compared their experimental data using a fitting parameter in above equation..E are defined in ref [110]. Kim and Lee [62]. 62.

76 - .3) where T1 and T2 are barrier transmittances and φ is the phase acquired by a wave in one round trip between the barriers. Whereas. Thus. the two terminal conductance [153] is found to be G = 2e T23 T31 ⎤ ⎡ T12 + h ⎢ T32 + T31 ⎥ ⎣ ⎦ 2 (5. The first term in bracket T12 describes direct elastic transmission between leads 1 and 2 whereas second term accounts for the inelastic transitions. The conductance derived by considering phase difference between various multiple reflections is given by Landauer formula [16]. An exact . the role of direct transmission and multiple reflections has not come in the formulation. The most popularly used formula in this respect was given by Landauer [155]. in Landauer-Büttiker formalism. it is based on certain assumption of fictitious lead in the Büttiker formulation. Although the analytical formulation by Kim and Lee [62] gives transmission coefficient while calculation of tunneling lifetime.4) where Tij is transmission coefficient from lead j to lead i. LandauerBüttiker formula clearly separates the directly elastic tunneling and multiple reflection terms in the conductance. G=e T1 T2 h 1 + (1 − T1 )(1 − T2 ) − 2[(1 − T1 )(1 − T2 )]1 2 cos ϕ 2 (5.Chapter 5: Electron transport through DBQW & explanation of universal phase behavior been calculated by Wulf et al [154] by employing the R-matrix formulation. However.

2 Transmission coefficient in terms of coupling coefficients ψ1f ψ1r ψ2 V1 ψ3 ψ4 ψ5f V2 U -a1 0 L L+a2 Figure 5.2 Schematic diagram of QD as tunnel device modeled as a double barrier quantum well system .77 - .Chapter 5: Electron transport through DBQW & explanation of universal phase behavior mathematical expression without any assumption is derived in the following section which clearly separations the direct transmission and multiple reflections in the transmission coefficient. 5.

0 ≤ x≤ L L ≤ x ≤ a2 − a2 ≤ x ≤ ∞ (5.2 using the wave functions. . T2 =η 2 ⎢ −α a − i θ ' ⎢e 2 2 2 ⎣ 4⎦ ⎣ 5⎦ ⎣ (5.7) ⎡ −α 2 a2 + i θ2' ⎡ A5 ⎤ ⎡ A4 ⎤ ' e ⎢ B ⎥ = T2 ⎢ B ⎥ .6) where transmittances are ⎡ A2 ⎤ ⎡ A1 ⎤ ⎢ B ⎥ = T1 ⎢ B ⎥ . ψ 1r = B1 e αx − ik1 ( x + a1 ) . − ∞ ≤ x ≤ − a1 . − a1 ≤ x ≤ 0 . Therefore. T1 = η1 ⎣ 2⎦ ⎣ 1⎦ ⎡e −α1 a1 − iθ1 ⎢ α a + iθ ⎢e 1 1 1 ⎣ e −α1 a1 + iθ1 ⎤ ⎥ eα1 a1 − iθ1 ⎥ ⎦ eα 2 a2 − i θ2 ⎤ ⎥ ' α 2 a2 + i θ 2 ⎥ e ⎦ ' (5. we have solved the Schrödinger’s equation for double barrier quantum well system shown in figure 5. .Chapter 5: Electron transport through DBQW & explanation of universal phase behavior Separation of various terms involved in the direct and multiple reflections within QW is crucial in understanding the basic physics of coherent transport through it.5) ψ 2 = A2 e 1 + B2 e 1 ψ 3 = A3 cos k 2 x + B3 sin k 2 x ψ 4 = A4 e −α 2 ( x − L ) −α x + B4 e α 2 ( x− L ) ψ 5 f = A5 e ik1 ( x − L − a2 ) We find that the matrices for the forward transfer are given by ⎡ A5 ⎤ ⎢ B ⎥ = T2 Q T1 ⎣ 5⎦ ⎡ A1 ⎤ ⎢B ⎥ ⎣ 1⎦ (5. ψ 1 f = A1 e ik1 ( x + a1 ) .8) and the forward coupling matrices are .78 - .

ηi = 1 + 2 2 2 k1 αi θ i = tan −1 αi k1 = (5.79 - . 2 h k1 = However.13) (5.12) 2 m( E − U ) 2mE .9) Here.11) π π θ = − (θ1 + θ 2 ) . the various terms involved are α i2 k12 1 ' 1 ηi = 1 + 2 . it is more convenient to use inverse matrices ⎡ A1 ⎤ −1 −1 ⎢ B ⎥ = T1 C T2 ⎣ 1⎦ ⎡ A5 ⎤ ⎢B ⎥ ⎣ 5⎦ (5.Chapter 5: Electron transport through DBQW & explanation of universal phase behavior 1⎛ α ⎞ Q11 = ⎜1 + 1 ⎟ cos k 2 L + 2 ⎜ α2 ⎟ ⎠ ⎝ 1⎛ α ⎞ Q22 = ⎜1 + 1 ⎟ cos k 2 L − 2 ⎜ α2 ⎟ ⎠ ⎝ 1⎛ α ⎞ Q12 = ⎜1 − 1 ⎟ cos k 2 L + 2 ⎜ α2 ⎟ ⎝ ⎠ 1⎛ α ⎞ Q21 = ⎜1 − 1 ⎟ cos k 2 L − 2 ⎜ α2 ⎟ ⎝ ⎠ 1 ⎛ k 2 α1 ⎞ ⎜ − ⎟ sin k 2 L 2 ⎜ α 2 k2 ⎟ ⎝ ⎠ 1 ⎛ k 2 α1 ⎞ ⎜ − ⎟ sin k 2 L 2 ⎜ α 2 k2 ⎟ ⎠ ⎝ 1 ⎛ k 2 α1 ⎞ ⎜ + ⎟ sin k 2 L 2 ⎜ α 2 k2 ⎟ ⎝ ⎠ 1 ⎛ k 2 α1 ⎞ ⎜ + ⎟ sin k 2 L 2 ⎜ α 2 k2 ⎟ ⎝ ⎠ (5.10) π 2 −θ i' . θ i' = tan −1 αi k1 (5. k2 = h h 2m (Vi − E ) and α i = with i =1.14) where the barrier transfer matrices . θ ' = − (θ1 − θ 2 ) 2 2 and (5.

80 - .16) are important in explaining the electron transport through QD. ' −α 1 a1 + i θ1 ⎥ e ⎦ ' ⎡e T2−1 =η 2 ⎢ −α a + i θ ⎢e 2 2 2 ⎣ and coupling matrices α 2 a2 − i θ 2 ⎤ ⎥ e −α 2 a 2 − i θ 2 ⎥ ⎦ e α a2 + i θ 2 (5.18) . t= t1 t 2 ⎡C + C −2α1a1 −2α 2a2 −2iθ + C −2α1a1 −i (θ +θ ' ) + C −2α 2a2 +i (θ ' −θ ) ⎤ 22 e 12 e 21 e ⎢ 11 ⎥ ⎣ ⎦ (5. using these inter-relations we can write the transmission coefficient as.Chapter 5: Electron transport through DBQW & explanation of universal phase behavior T1−1 ⎡eα1 a1 + i θ1' =η ⎢ ' ⎢eα1 a1 − i θ1 ⎣ ' 1 e −α1 a1 − i θ1 ⎤ ⎥ .17) with t1 = e ' −α1a1 −iθ1 η1' and t2 = e −α 2 a2 +iθ 2 η2 (5. Now.15) 1⎛ α ⎞ C11 = ⎜1 + 2 ⎟ cos k 2 L − 2 ⎜ α1 ⎟ ⎠ ⎝ 1 ⎛ k2 α 2 ⎞ ⎜ − ⎟ sin k 2 L 2 ⎜ α1 k 2 ⎟ ⎝ ⎠ α ⎞ 1⎛ α ⎞ 1⎛ k C 22 = ⎜1 + 2 ⎟ cos k 2 L + ⎜ 2 − 2 ⎟ sin k 2 L 2 ⎜ α1 ⎟ 2 ⎜ α1 k 2 ⎟ ⎝ ⎠ ⎝ ⎠ 1⎛ α ⎞ C12 = ⎜1 − 2 ⎟ cos k 2 L − 2 ⎜ α1 ⎟ ⎝ ⎠ 1⎛ α ⎞ C 21 = ⎜1 − 2 ⎟ cos k 2 L + 2 ⎜ α1 ⎟ ⎝ ⎠ 1 ⎛ k2 α 2 ⎞ ⎜ + ⎟ sin k 2 L 2 ⎜ α1 k 2 ⎟ ⎝ ⎠ 1 ⎛ k2 α 2 ⎞ ⎜ + ⎟ sin k 2 L 2 ⎜ α1 k 2 ⎟ ⎝ ⎠ (5.

Magnitude and phase of t for a typical AlGaAs system is shown in figure 5. The phase of this conventional t evolves continuously by π for each conductance cycle without a phase slip in-between . Figure 5.3.Chapter 5: Electron transport through DBQW & explanation of universal phase behavior where t1 and t2 give the coefficients for direct transmission through barriers.17) gives the conventional transmission coefficient for which phase of t evolves continuously by π for each transmission cycle.81 - .3 Magnitude and phase of t plotted against k2L. However. Equation (5.

which is actually three .Chapter 5: Electron transport through DBQW & explanation of universal phase behavior it is not in agreement with the experimental observations shown in figures 1.20) gives the contribution arising due to multiple reflections.82 - .7 and 5. 5.19) can be retained even in a QD. t 0 ≡ t1 t 2 = (C11 + M ) t where M = C 22 (5. Therefore. so that the tunnel component can be written as.17) is required.19) superimpose linearly because of the dimensional restriction so that they are completely aligned and will give the conventional result. In the standard one dimensional problem.1..3 Separation of coherent and sequential tunneling coefficients and explanation of universal phase behavior in coherent transport A closer look at bracketed terms in the denominator of this equation shows that all the four terms have distinct origins. While the properties of the first term in equation (5. the two terms in equation (5. which show a sharp phase slip of π at the transmission minima [37-38]. a re-interpretation of the equation (5.19) e − 2 α 1a1 − 2 α 2 a 2 − 2 i θ + C 12 e − 2 α 1a1 − i (θ +θ ' ) + C 21 e − 2 α 2 a 2 + i ( θ ' −θ ) (5.

Chapter 5: Electron transport through DBQW & explanation of universal phase behavior dimensional but for which one dimensional transmission has been assumed in the direction of the incident wave. it will be more appropriate to consider components arising due to the various terms as orthogonal to each other allowing us to replace M in equation (5.83 - . Further. such an alignment is not always possible for the multiple reflection terms contained in M. The alignment is disturbed as one moves from small size QD to larger ones.21) Now. as discussed by Büttiker [153].22) . t0 can be treated as a vector with two orthogonal components.19) by an orthogonal term δ = 2 C12 e − 2α1a1 − i (θ +θ ' ) 2 2 + C 21 e − 2α 2 a2 + i (θ ' −θ ) 2 2 + C 22 e − 2α1a1 − 2α 2 a 2 − 2iθ 2 2 2 2 = C12 η1't1 + C21 η2t2 + C22 η1't1η 2t2 4 4 2 (5.19) to interact coherently with the first one. linear superposition of the three terms of M may not be possible and these terms may behave independent of each other. Further. In such a situation. t 0C = C11 2 C11 +δ 2 t0 (5. one corresponding to the coherent transmission given by. Thus. in semiconductor devices there is a possibility of incoherence introduced by collisions which should here include reflections from interfaces. for large size QDs it may not be possible for the second term of equation (5.

27) gives the eigenstates of the system.25) tS = δ 2 C11 +δ 2 t (5. t0 S = so that. When the same system is closed by extending the external boundaries to ± ∞ the roots of the equation 1⎛ α ⎞ C11 ≡ ⎜1 + 2 ⎟ cos k 2 L − 2 ⎜ α1 ⎟ ⎝ ⎠ 1 ⎛ k2 α 2 ⎞ ⎜ − ⎟ sin k 2 L = 0 2 ⎜ α1 k 2 ⎟ ⎝ ⎠ (5. δ 2 C11 +δ 2 t0 (5.26) It is to be noted that so far. The coupling coefficient changes its sign around the zeros of C11 which is . tC = and C11 2 C11 + δ 2 t (5.23) 2 2 2 t 0 = t 0C + t 0 S (5.Chapter 5: Electron transport through DBQW & explanation of universal phase behavior and the other due to sequential tunneling. we have been dealing with an open system.84 - . zeros of C11 give the eigenstates for a closed system and the same is crucial in separating tS from tC.24) The two terms t0C and t0S may give independent transmission coefficients at the output given by. given by. Thus.

The difference in the line shape and the sharpness of phase evolution as one move from few electron occupancy to higher occupancy is noteworthy. the coupling changes from symmetric to antisymmetric or vice versa around this position which corresponds to crossover of occupation probability as shown in figure 4.Chapter 5: Electron transport through DBQW & explanation of universal phase behavior justified in view of the fact that for a closed system e.4 Magnitudes and phases of the coherent tunneling coefficient tC and sequential tunneling coefficient tS are plotted against k2L for a QW with L=100nm. a1=a2=2nm. V1=V2= 450meV. an asymmetric double quantum well system.85 - .2. . Figure 5. E= 430meV and m*= 0..g.0665mo. The trends for tC are in agreement with experimental results of ref [38] (Figures 3b and 3c) and hence explain the universal phase evolution including the phase slip at conductance zeros.

It should be noted that the transmission peaks broaden as one moves to higher values of k2L and hence. we have plotted magnitude and phase of tC by increasing barrier width to a1=a2= 5nm in figure 5. This essentially means that a resonant tunneling peak is composed of two parts. thus transmission breaks in two independent components tC and tS so that the net transmission probability | t |2 is sum of | tC |2 and | tS |2. In any experiment. In figure 5. in which tS is properly filtered out. explains the universal phase evolution including the phase slip at the minimum of | tC |2.5(a) and an asymmetry of barriers introduced by taking a1=2nm and a2=5nm in figure 5. higher electron occupancy.86 - . To study the effect of variation in barrier width. our conclusions are similar to those arrived at by Büttiker with respect to coherent and sequential tunneling [153]. In this regard.Chapter 5: Electron transport through DBQW & explanation of universal phase behavior In a QD. These calculations clearly show that the phase slip at conductance zero and phase evolution by π in each conductance cycle is a . of which only one travels coherently. The figure clearly shows that the trends of magnitude and phase of tC are complete agreement with experimental results of ref [38] and thus.5(b).4. one can clearly observe a phase slip at conductance zero and each cycle evolving in phase. magnitude and phase of tC and tS are plotted for a QD with symmetric barriers with a1 = a2 = 2nm.

Figure 5. we have plotted | t |2. | tC |2 and | tS |2 in figure 5.6 for a typical transmission peak.Chapter 5: Electron transport through DBQW & explanation of universal phase behavior universal feature of coherent transmission. This clearly . To further our understanding of transmission process. These trends of are in agreement with experimental results. in all cases the phase evolution is during the transmission peaks which become sharper for higher barrier width. However. The effect of increasing barrier width is to make the resonant peak sharper by suppressing the transmission in the valley region.87 - .5 Magnitudes and phases of the coherent tunneling coefficient tC are plotted for (a) weak coupling with a1=a2= 5nm and (b) barrier asymmetry with a1= 2nm and a2=5nm.

88 - . Thus. In any system in which this separation has not occurred completely. a continuous phase evolution or a mixed mode may be observed. sequential tunneling coefficient tS and resonant tunneling coefficient t are plotted to show that t is composed of tC and tS. in which for smaller QD with few electron occupancies the phase slip of π has not always been observed. Separating the sequential part from the coherent one is key to the observed universal phase evolution. . their curvatures all may play important role in separating tS from tC and giving rise to the observed universal phase evolution.Chapter 5: Electron transport through DBQW & explanation of universal phase behavior shows that a resonant transmission comprises of a coherent part and a sequential part. roughness of the barrier surfaces.6 Transmission probabilities of coherent tunneling coefficient tC. the size of the QD. Figure 5. This seems to be the case with the experimental results of Avinum-Kalish [37].

89 - . At this position. one corresponding to the density of states of the QBS and the other for remaining free space.28) where K is a proportionality constant. in the simplest terms Γ= τ h ≈ K | t1 |2 + | t 2 |2 { } (5. Γ depends on | t1 |2 and | t2 |2 almost in the same way as δ does in our formulation given by equation (5. The fractional occupancy of the QBS is given by 2 δ 2 (C11 + δ 2 ) .Chapter 5: Electron transport through DBQW & explanation of universal phase behavior It is to be noted that all the peaks are displaced from the position of the eigenstates for the closed system occurring at C11 = 0.21) except for a double reflection term which gets included here due to . It is also worth a mention that the explanation given in terms of BreitWigner [152] formula applies directly to the sequential part of tunneling with Γ/2 having the same significance as δ in our formulation. The line width Γ varies inversely with lifetime τ of QBS. The entire renormalization process of t0 seems to divide the phase space in two parts. a coherent transmission is essentially through the free space available for transfer of electrons whereas the sequential tunnelng is through the QBS. | tC |2 becomes zero whereas tS and t may have finite values. Thus. The lifetime τ in turn depends upon the tunneling probabilities | t1 |2 and | t2 |2 and therefore. Thus.

From the above discussions. 5. we also find that in coherent transmission the tunnel barriers act in series with amplitude of the wave dropping by a fixed amount at each barrier. .4 Conclusions We have obtained exact formulae for transmission coefficient through a double barrier quantum well in which various multiple reflection terms are separable. the coherent transmission is switched off allowing for a phase slip and hence. whereas the sequential tunneling takes into account the leakage from both barriers acting in parallel as is clear from expression for δ as well as Γ. we have been able to separate the coherent and sequential tunneling coefficients and find that the coherent tunneling coefficient shows a universal phase evolution with phase slip at zeros of the coherent tunnel amplitude and all the coherent conductance peaks evolve in phase with each other. a reset of the system for a new conductance cycle.90 - .Chapter 5: Electron transport through DBQW & explanation of universal phase behavior multiple reflections. This further shows that at the quantum resonance position (at C11 = 0). By doing so.

70]. 111. due to it’s indirect band gap was never considered useful material for light emitting devices until the discovery of porous silicon in which due to quantum confinement light emission of practical use could be obtained [64-65.Chapter 6 Nonradiative recombinations in nanosized semiconductors 6. Though. 118] and much work has been done on optical transitions and spectral analysis [65-69]. it has been well established that an increased optical efficiency of nano-sized semiconductors as compared to bulk material is due to quantum confinement [44. The nonradiative processes compete with . 64.1 Introduction Nanocrystalline and microcrystalline semiconductors have found wide applications in optoelectronic devices because of their increased optical emission efficiencies compared to bulk materials [64-65. 156]. little attention has been given to nonradiative recombination processes [40. Particularly silicon. 66] and increased oscillator strength [116. 156].

we evaluate the effect of finite size of the surrounding medium (semiconductor) on the rate of recombination.Chapter 6: Nonradiative recombinations in nano-sized semiconductors radiative ones and it is their relative magnitude that decides the efficiency of light emission [43. This leads to enhanced optical efficiency in micro and nanosized semiconductors. enhances the radiative processes. Quantum mechanical effects [157] arising in the charge transport due to size reduction have been neglected in this first order theory. A free electron moving in the surrounding space is captured by an empty trap (nonradiative recombination centre) which can subsequently capture a free hole. In this paper.92 - . the surface to volume ratio increases and recombination is more likely to occur at the surface rather than the bulk. similar conclusions can be drawn for bulk . As the size of the grain reduces. For this reason. 6. We show here by a first order theory that small grain size suppresses the nonradiative recombination and hence. The model presented here is based on the assumption that effective mass approximation remains valid for smaller size grains and is invariant under size reduction.2 Calculation of Surface recombination velocity Nonradiative recombinations usually proceed via a localized trap [158]. we analyse the effect of finite grain size on surface recombination velocity. 48]. as the size is decreased. However.

The solid angle subtended by the surface element dS on the volume element dV for configuration shown in figure 6. Of these.3) Further. The capture event can be described as follows: Free electrons (or free holes) are scattered continuously in all directions due to the various collision processes in the semiconductor. if λ is the mean free path of the electrons. Total outward flux from the volume element dV is n τ dV (6. which has been assumed to be uniform and τ is the mean collision time. the probability of electrons starting from dV to reach dS uninterrupted is e − r λ .Chapter 6: Nonradiative recombinations in nano-sized semiconductors lifetime. the electrons which are directed towards a surface element can be captured provided they don’t meet a second collision in the path. a scattering centre in a volume sends electrons in all directions.93 - .1. is dS cosθ / r 2 (6. Thus. the flux of the electrons reaching the surface element dS from volume element dV is .2) The flux of electrons directed from volume element dV to surface element dS is dS cosθ n dV 4πr 2 τ (6.1) If n is the density of electrons in the bulk semiconductor. Thus.

Chapter 6: Nonradiative recombinations in nano-sized semiconductors −r e λ dS cosθ n dV 4πr 2 τ (6.1 A surface element dS in a semiconductor of semi-infinite geometry This when integrated over the entire volume of the semiconductor gives the flux of the electron reaching the surface element dS.94 - . − r cosθ n ⎤ ⎡ dV ⎥ dS dφ = ⎢ ∫∫∫ e λ 4πr 2 τ ⎣ ⎦ (6.5) and we have (6.6) If vth is the average thermal velocity of electrons then λ = vthτ − r cosθ n ⎡ ⎤ dV ⎥ dS dφ = vth ⎢ ∫∫∫ e λ 2 4πr λ ⎣ ⎦ .4) dV = r2 sinθ drdθdφ r θ dS Figure 6.

Chapter 6: Nonradiative recombinations in nano-sized semiconductors Let us now define by vR the average of the normal component of the velocity with which electrons of density n are reaching the surface element dS.2.9) Since. For this case. we have ∞ vR = vth ∞ π 2 2π r =0 θ =0 ϕ =0 ∫ ∫ ∫ e −r cosθ 2 r sin θ dθdϕdr λ 4πr 2 λ (6. 2 ϕ = 2π ϕ =0 ∫ dϕ = 2π r =∞ and r =0 ∫e −r λ dr = λ (6.7) (6. θ =π 2 θ =0 ∫ 1 cosθ sin θ dθ = .1 Semi-infinite Geometry Let us now calculate vR for a semi-infinite geometry. we get ∞ vR = vth 4 (6.95 - .8) 6.10) Calculating integrals.11) . so that dφ = n v R dS which gives ⎤ ⎡ e − r λ cosθ v R = vth ⎢ ∫∫∫ dV ⎥ λ 4πr 2 ⎥ ⎢ ⎦ ⎣ (6.

12) Integrating for φ.2 Semi-conductor Slab of finite thickness Now. we introduce confinement in the problem.96 - . For a non-degenerate electron gas vth = 8 KT π m and therefore ∞ v R = KT 2 π m which has the same meaning as used in thermionic emission theory [159]. For this case the limits of integration on r for a given θ will be from 0 to W cosθ . we get . on solving the integrals.13) Normalizing r ≡ r / λ and letting cosθ = x.2.Chapter 6: Nonradiative recombinations in nano-sized semiconductors ∞ Where vR is the average of normal component of velocity with which electrons are received at the surface element dS in a semi-infinite geometry. vW R = vth π / 2 W / Cosθ 2π θ =0 ∫ r =0 ∫ ∫ e−r / λ λ ϕ =0 cosθ 2 r sinθ dθ d ϕ dr 4π r 2 (6. 6. vW R vth π / 2 W / Cosθ e − r / λ = dr cosθ d(cosθ ) 2 θ ∫0 r ∫0 λ = = (6. we get vW R v = th 2 −r ∫ ∫e 1 W /x dr x d x (6. This gives. For this let us consider a semiconducting slab with electrons confined between surfaces at z=0 and z=W.14) x = 0 r =0 Now.

16) and therefore.2.Chapter 6: Nonradiative recombinations in nano-sized semiconductors ∞ vW = β v R R (6. the effect of space confinement is to reduce the contribution of bulk semiconductors in the flux of electrons reaching the surface element. However.2.x ⎠ (6. contribution of bulk in the flux of electrons reaching dS. the confinement itself is due to the presence of another surface at a perpendicular distance W from the element dS. exp⎜ − ⎟ dx ⎝ λ . 6.1 Contribution from Surface To calculate the contribution of the surface let us consider a surface element dA as shown in figure 6. it will reflect (re-emit) a fraction of the electron flux incident on it. If this surface is not completely absorbing.18) .17) Thus.2.97 - .15) with β =1 − 2 x =0 ∫ 1 ⎛ W ⎞ x . Solid angle subtended by surface element dS at the surface element dA is dS cosθ 4πr 2 (6. W ∞ dφ B = n vW dS = β n v R dS R (6.

Chapter 6: Nonradiative recombinations in nano-sized semiconductors If εn is the emissivity of the surface and cos α is the direction cosine of the surface element dA with respect to vector r then flux of the electrons from dA for a diffused emission towards dS is given by → ε n cos θ dA Now. the flux of electron reaching dS will be (6.20) dA dA = r dθ.19) εn e −r λ cosθ cosα dS dA π r2 (6.21) .98 - .2 Configurations for capture at surface element dS (a) from a general surface element dA and (b) for a slab of thickness W The flux received by the element dS from the entire surface is obtained by integrating the above expression on the surface element dA and it is given by dφ S = ∫∫ ε n e −r λ Cosθ Cosα dS dA π r2 (6. r tanθ dϕ W cosθ α r θ dS r= α W θ dS r tanθ (a) (b) Figure 6.

they will capture electrons and may hold them for sufficient time to allow the subsequent capture of holes so that recombination takes .Chapter 6: Nonradiative recombinations in nano-sized semiconductors For an element dA on a plan surface at a distance W.24) We note that depending on emissivity. φ). W dφ S = (1 − β )ε n dS (6. W → ∞ and W W dφ S is zero. we note that a surface has a large number of deep as well as shallow traps.21) and by noting that for the geometry under consideration α and θ are equal. integrating for φ and r and substituting cosθ = x. x ⎟ dx ⎥ dS ⎟ ⎝ ⎠ ⎦ ⎣ 0 (6. exp⎜ − ⎜ λ . As confinement increases. The deep traps are the recombination centers and if these are empty. we get.22) Upon putting this value of dA in equation (6. dφ W S ⎡ 1 ⎛ W ⎞ ⎤ = ε n ⎢ 2 ∫ x . the contribution from surface is complementary to that from bulk. Now.23) which gives.99 - . For this. W reduces and dφ S starts increasing. For a semi-infinite geometry. it remains for us to relate emissivity of the surface with the flux incident on it. with angular positions (θ. we have dA = rdθ r tan θ dϕ = W dθ W tan θ dϕ cos 2 θ (6.

All these processes can be lumped together in terms of reflection coefficient fr which is assumed to be arising mostly due to diffused reflectance / re-emission.25) However. a large portion of the surface may have shallow traps at which electrons are captured and are re-emitted very effectively. the capture in deep states is through a cascade process. ε n = f r n vr = (1 − f a ) n v R (6. we can define by fa the probability of the electron sticking to the surface. Further. in which it is first absorbed in excited state and then falls to ground state. However. as explained by Lax [160]. we have f a + f r + f t =1 (6.26) The rate of recombination at the surface in terms of sticking probility is given by dR = f a dφ (6. Thus. ft can be assumed to negligible and we have fr = 1 – fa and therefore. the surface element dA may reflect back the carriers due to surface barriers. The charge conservation may require a third term ft for transport of carriers from one grain to another. Thus. Thus. fa is different for different types of traps present on the surface. surface acts as a secondary source of electrons.27) . Also.Chapter 6: Nonradiative recombinations in nano-sized semiconductors place. if we neglect inter-granular transport.100 - .

28) Now.28) we get. ∞ n v R dS = n β v R dS + (1 − f a )(1 − β ) n v R dS (6.7).24) we get. W dφ S = (1 − f a ) (1 − β ) n v R dS (6. On substituting the value of εn in equation (5.29) By using equations (5.17) and (5. it will be zero. we note that the total flux reaching the surface is dφ = dφ B + dφ S (6. The actual value of fa will vary between 0 and 1. For a completely absorbing surface fa is unity whereas for a completely reflecting surface with no recombination centers on it. for a highly disordered surface.101 - . If Nti is density of the surface recombination centers of capture cross-section σi then for low density of the traps f a ≈ ∑ N tiσ i . However. (6. isolation of i the traps assumed in the above summation may not be valid and one has to assume an effective value of fa which will always be less than unity.Chapter 6: Nonradiative recombinations in nano-sized semiconductors The sticking probability fa for the surface denotes the capability of the surface element to absorb the electron.31) .30) so that vR = 1− (1 − f a )(1 − β ) β ∞ vR (6.

Chapter 6: Nonradiative recombinations in nano-sized semiconductors

The above equation shows that confinement reduces vR through absorptivity of the surface fa. However, for a perfectly re-emitting surface,
∞ [vR ] f →0 = v R = vth
a

4 . This is a statement of conservation of charge and

proves the consistency of the calculations. It is the absorptivity of the surface introduced for confinement that limits the flux reaching the surface element
dS and reduces the value of vR.
6.2.2.2 Surface recombination velocity

If SR is the surface recombination velocity, the rate of recombination at the surface element dS can be written as,
dR = S R n dS

(6.32)

This by using equating equation (6.7) and (6.27) give
S R = f a vR

(6.33)

Thus, the surface recombination velocity is product of the velocity vR with which the electrons reach the surface and their sticking probability fa. In
∞ terms of v R the surface recombination velocity becomes

SR =

fa β ∞ vR 1− (1 − f a )(1 − β )

(6.34)

- 102 -

Chapter 6: Nonradiative recombinations in nano-sized semiconductors

which can be further simplified to give
∞ S R = vR

⎡1 1 ⎤ ⎢ f + β − 1⎥ ⎣ a ⎦

−1

(6.35)

Thus, we note from above expression that surface recombination velocity SR is highest for a semi-infinite system with perfectly absorbing
∞ surface and it’s value is given by v R (= vth 4) . This is the velocity with

which an infinite sink will absorb the particles arriving at it. Reduction in either fa or β reduces the value of SR. The reduction in fa is due to reemission from the surface, whereas reduction in β will arise if the space provided for electrons to move is reduced from semi-infinite to a finite geometry. The above equation clearly brings out the effect of confinement on surface recombination velocity.
6.2.3 Cylindrical grain

From equation (6.24), we note that the contribution arising from emissions from the surface is complementary to that from the bulk. Irrespective of the geometry, equations (6.24) to (6.35) are based on the basic principle of space confinement and therefore, apply to all types of configurations. Thus, equation (6.35) can be applied to other geometries also provided the weight factor β for the flux coming from the bulk is known. As

- 103 -

Chapter 6: Nonradiative recombinations in nano-sized semiconductors

an attempt to extrapolate equation (6.35) to other geometries, we derive the expression for β using cylindrical geometry shown in figure 6.3. Such a situation may typically arise in semiconductor wires like those in porous silicon. The surface element is located at the origin of the cylindrical coordinate system. For a grain of diameter D,
D vR

= vth

z = − ∞ϕ = 0 ρ = 0

∫ ∫ ∫

π

D Sinϕ

e−r / λ
λ

cosθ sin ϕ ρd ϕ dρ dz 4π r 2

(6.36)

z ρ 90° θ r

dV = ρ dρdφdz

D
ρ φ

dS

z

dS

(a)

(b)

Figure 6.3 (a) Configuration for a trap at the surface of cylindrical semiconductor column. (b) Cross-sectional view of this configuration

- 104 -

we use typical values for silicon.38) with β1 = 4 ∞ π / 2 D Sinϕ z =0 ϕ =0 ρ =0 π ∫ ∫ ∫ e − z2 +ρ 2 λ λ {z ρ sin ϕ 2 + ρ2 } 3/ 2 ρd ϕ dρ dz (6. We assume a deformation potential scattering dependent mean free path given by [161].105 - .39) The surface recombination velocity SR for this case can be calculated by replacing β by β1 in equation (6. πh 4 cl λ = 2 2 m ε k BT (6.3 Discussion and conclusions To illustrate the effect of confinement.Chapter 6: Nonradiative recombinations in nano-sized semiconductors The factor sinφ in above equation arises due to the cylindrical geometry considered here. ∞ D v R = β1 v R (6. 6. we find that. we obtain.35).37) On substituting these values. From the geometry shown in figure 6. wherein the normal to dS makes an angle (π/2 – φ) with the ρ – z plane. r = z2 + ρ 2 and Cosθ = ρ z +ρ 2 2 (6.4.40) .

..0 fa=0.1 10 100 W (nm) Figure 6.7 fa=0. 77K fa=1..Chapter 6: Nonradiative recombinations in nano-sized semiconductors 1.8 _____ 300K …..2 0.9 fa=0.3 fa=0.106 - .27) for a semiconductor slab for different values of sticking probility fa is plotted against thickness W of the slab for silicon at temperatures 300K and 77K.0 fa=0..4 0.6 ∞ vR 0.0 0.4 Surface recombination velocity SR as given by equation (5.5 SR 0..

5 0. 77K fa=0.7 fa=1.7 fa=0.4 fa=0.2 fa=0.27) is plotted against diameter of cylinder D using β1 as given by equation (5.6 ____ 300K …….0 fa=0.0 0.Chapter 6: Nonradiative recombinations in nano-sized semiconductors 1.31). Surface recombination velocity SR as given by equation (5. Results presented here are for silicon at 77K and 300K for different values of fa. .5 For a semiconductor cylindrical column.5 fa=0.0 fa=0.3 0.9 fa=1.107 - .1 1 10 100 D (nm) Figure 6.0 fa=0.9 fa=0.1 SR v ∞ R 0.3 fa=0.8 0.

4 ×10 −5 λ= m T (6. the decrease in the size of grain reduces the capture rate from the bulk and the effect is more pronounced at lower temperature. In the case of cylindrical grain also. Also. Figure 6.4 as a function of thickness W for some typical values of sticking probability fa at 300K and 77K.35) are plotted in Figure 6. the . As is clear from the diagram.5 shows values of SR for a cylindrical grain calculated by using equation (6.35) with β replaced by β1 as given by equation (6. This applies both to the semiconductor quantum wires like those in porous silicon and semiconductor slabs in superlattices.41) The values of surface recombination velocity SR for a semiconductor slab given by equation (6. though we have confined our calculations to surfaces. Thus.108 - . Similar expressions can be obtained with somewhat more involved geometry for quantum dots with basic conclusions remaining the same. the surface recombination velocity reduces with decrease in grain size and a much more pronounced effect is observed at lower temperatures. reduction in the size of the semiconductor has a direct bearing on the efficiency of light emitters which show better performance when reduced to nanoparticle size.Chapter 6: Nonradiative recombinations in nano-sized semiconductors which upon putting values of constants for silicon give 1.39) for silicon at 300K and 77K.

This will further reduce the nonradiative recombination making these semiconductors more efficient emitters of light. the traps have many excited states and recombination is usually through a cascade process [160]. Quantum confinement may give rise to additional factors which have not been included here. . we have brought out the effects which have to be incorporated in the Shockley Read Hall model of recombination. if one wants to use it for small size grains. In this paper. As the size of the semiconductor is reduced to quantum size.109 - . We may point out here that in our calculations. we have assumed a constant capture cross-section. these excited states may disappear and may result in drastic reduction in capture cross-section. In actual situation.Chapter 6: Nonradiative recombinations in nano-sized semiconductors conclusions are of general nature and will apply to bulk traps as well.

confining potentials. The formulation accommodates all ADQW parameters such as QW widths. the field is quite challenging and there is a great upsurge in the novel application of new and exciting phenomenon reported in recent times. effective mass jumps etc. We find that. QW separation. The survey of literature on transport and recombination in nanosized semiconductors has been presented in the first chapter.Chapter 7 Summary and Conclusions This chapter presents a summary of the thesis and important conclusions drawn therein. first principle based analytical expressions have been derived in Chapter 2 for ADQW system. the survey clearly brings out the need of exact quantitative understanding of transport and recombination phenomenon so as to fully exploit the quantum properties of nanosized semiconductors. However. In order to study eigenstates of coupled QWs. The effect of .

Some of the applications of these analytical formulae have been discussed for GaAs / AlXGa1-XAs semiconductor heterostructures. However. The strong localization behavior of the eigenstates of the individual QW is clearly an ADQW feature. It is shown that for every QW for a given eigenstate another . it is shown that variation in alloy composition can also be resorted for transport optimization between QWs. Further. corresponding to minimization of asymmetry and ADQW behaving like a SDQW for this state. missing in SDQW.111 - . localization is decreased for strong coupling strengths. It is found that the effect of asymmetry can be minimized for a particular eigenstate by varying QW width and / or confining potential so that probability density in two coupled QWs becomes nearly equal for that energy level which in turn results in an efficient transfer of electrons.Chapter 7: Summary and Conclusions strength of coupling upon eigenvalues calculated using the analytical formula is found to be in agreement with those reported in literature by using numerical methods. The effect of varying confining potential for transport optimization is shown to be identical to that obtained by applying an electric field. In Chapter 3. a detailed study of the effect of coupling strength upon the eigenstates has been presented using the analytical formulae derived in the Chapter 2. This occurs at the minimum energy difference between the eigenstate under consideration and its nearest state.

This new type of coupling may find important applications in nano-electronic devices for loss less elastic transport. Further. The universality of this zero perturbation condition has been proved analytically as well as graphically and is found to meet with whenever the coupled QW has appropriate width and depth so that phase traveled by an electron wave through it is an integral multiple of π. the detailed study of charge transfer in coupled QWs has been presented in the Chapter 4. applications sensitive to interfacial disorders or coupling strength etc. In continuation of Chapter 2.Chapter 7: Summary and Conclusions QW can always be found which is completely matched with the host irrespective of coupling strength and electron can tunnel from the host to the guest without perturbing the former. the matched coupling described above is applicable to multiple QWs where a host QW can be coupled to as many QWs as required and none of them will disturb the original eigenstate. the entire mechanism of electron transfer . The probability crossovers are shown to be around the minimum of the energy separation between the two nearest energy states. At this probability crossover position.112 - . applications having monochromaticity requirements. It is found that determination of fractional occupancies of finding electron in the two QWs is crucial for understanding the mechanism of charge transfer between coupled QWs and QDs. a position different from the energy crossover position on E-k2 scale.

Next. particularly . the eigenstate localized in the first QW is delocalized which are then localized sharply in the second QW and then get delocalized again to get localized in the first QW once again. The process of electron transfer involves one energy state being replaced by another of opposite parity and coupling changes alternatively between symmetric and anti-symmetric ones. The applications discussed in Chapter 2 and the new phenomena presented in Chapter 3 and 4 clearly reveal usefulness of analytical expressions for ADQW system derived in the Chapter 2.Chapter 7: Summary and Conclusions takes place. Increasing strength of coupling by reducing barrier width b increases ∆E as well as ∆k. although a simple correlation may not exist in this case. The process of charge transfer takes place in three steps. The width of the crossover is determined both by the strength of coupling and the asymmetry. In the first step. the entire spectrum of energy eigenstates gives an appearance of staircase type of picture in which each state goes down by one step around the crossover at which the occupation probability sharply changes their belonging from first QW to second QW and thus giving rise to a resonant effect.113 - . Varying L1 (or L2) may also change ∆k and ∆E. This describes the interplay between energy eigenstates of coupled QWs and the charging of individual QWs. each resonance corresponds to an electron transfer and the spectrum going down by one step.

Based on first principle semi-classical calculations. exact formula for transmission coefficient for a QD modeled as a double barrier quantum well has been obtained in which directly transmitting term and various multiple reflection terms are separable. The calculations result in a simple formula for surface recombination velocity as a function of sticking probability and geometry parameter.114 - . The calculation of surface recombination velocity as a function of size of the grain clearly shows that the decrease in the size of grain reduces the capture rate from the bulk and the effect is more pronounced at lower temperature. In the Chapter 5. Although. the enhanced optical efficiency in nanosized semiconductors have been explained in terms of suppression of nonradiative recombination in the Chapter 6. The coherent component in transmission coefficient is due to the direct tunneling component whereas the multiple reflection components give the sequential tunneling coefficient. where slab . this has been shown for confined slab and cylindrical grain.Chapter 7: Summary and Conclusions simplicity in use and effectiveness in accommodating various material parameters as well as in understanding the underlying basic physics of coupled QWs and QDs. The magnitude and phase of the coherent tunneling coefficient provide an explanation for the universal phase evolution including the phase slip at the zeros of coherent tunnel amplitude.

Thus. However. . suppression of nonradiative recombinations.Chapter 7: Summary and Conclusions resembling quantum well in superlattices and heterostructures and cylindrical grain resembling semiconductor quantum wires.115 - . reduction in the size of the semiconductor leads to reduction in capture rate at traps and therefore. These decreased nonradiative recombinations have a direct bearing on the efficiency of light emitters which show better performance when reduced to nano-particle size. the conclusions are of general nature and apply to nanosized cluster of arbitrary shape.

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*Corresponding author. Such studies have major implications on electronic. This condition shows a complete delocalization and the probability of finding the electron in the two QWs becomes equal. the problem finds direct applications in heterostructures. R. Results obtained are in agreement with those reported in the literature by numerical methods and do away with the need of perturbation approximation used in such cases. Jodhpur 342 001.3d [5. Jodhpur 342 011. Month?? 2006. optical. resulting in a splitting of the eigenstates. quantum computation [7].2006–5:36pm] (TPHM) [1–11] [First Proof] Philosophical Magazine. India (Received 21 January 2006. ??. The problem is solved in terms of an inversion plane at the centre of the barrier around which a transition occurs. No. Jai Narain Vyas University. single electron transistors [6]. 1–11 5 Analytical expressions for asymmetric double quantum wells and their application to semiconductor heterostructures JASA RAMy and S. which shows that the energy states of the individual wells couple themselves in two different ways. DHARIWAL*z yDefence Laboratory. Vol. once an asymmetry is introduced.New XML Template (2006) {TANDF_FPP}TPHM/TPHM_A_181481. and form a basis for the study of artificial molecules [9]. 1. The analysis shows that the coupled QWs can be matched for a given energy level to allow maximum transport between them by variation of one or more of these parameters so that the energy difference between it and the next nearest state is minimal. roots of which give energy eigenstates and enable derivation of corresponding wave functions. namely symmetric and anti-symmetric interactions. ?. Email: dhariwalsr@yahoo. The simplest is an asymmetric double quantum well (ADQW) through which all basic features of interacting nanostructures can be easily understood [1–3]. As an example. Solution of Schrodinger’s equation for a symmetric double quantum well ¨ (SDQW) with infinite outer boundaries is a textbook problem. such as lasers [4].co. memories. Introduction 25 30 35 Increasing demand of high density nano-sized quantum wells has resulted in extensive study of the mutual interaction of these systems. confining potential and material composition. India zDepartment of Physics.uk/journals DOI: 10.com Philosophical Magazine ISSN 1478–6435 print/ISSN 1478–6443 online ß 2006 Taylor & Francis http://www. quantum well (QW) width. in final form 13 May 2006) 10 15 20 Analytical solution of Schrodinger’s equation for an asymmetric double quantum ¨ well structure is obtained for the first time in terms of a transcendental equation. However. short wavelength light emission [5]. electro-absorption [8]. In addition.tandf. semiconductor devices.1080/14786430600815393 . which amounts to an asymmetric system becoming symmetric with respect to probability density.6. GaAs/AlxGa1ÀxAs system has been discussed with respect to variations in barrier width. dielectric and other material properties.

such a method can be applied when barrier width is sufficiently large and interaction is weak.6. the validity of which is limited to weakly interacting systems [3]. We have solved analytically the Schrodinger’s equation for an asymmetric double ¨ quantum well (ADQW) system. 2. The problem can be solved by a numerical iterative method as outlined by Kolbas and Holonyak [10]. However. Ram and S. L2 x < 1 ð2Þ 70 by matching the and (1/m*)d /dx at boundaries as per Ben Daniel-Duke conditions [18] at x ¼ ÀL1. Transcendental equation for ADQW system The time-independent Schrodinger’s equation: ¨ h "2 d2 ðxÞ þ ½E À Vðxފ ðxÞ ¼ 0 2mà dx2 65 ð1Þ is solved for the potentials and effective masses: 8 8 >0 > mb . Such numerical methods have been adopted by many workers [11. The solution finds direct applications in the design of electronic systems of practical interest. such an inversion plane disappears and simple explanation in terms of symmetric and anti-symmetric coupling is not applicable. whereas the probability function is assumed to tend to zero at x ! Æ1. À1 < x ÀL1 > > > > > > > V1 > m1 . Dhariwal 45 50 55 60 either in terms of well width or depth. 14]. which results in a much simplified mathematical formulation of the problem. which appeals to many. ÀL1 x 0 > > < < à m ¼ mb . which allows calculation of eigenstates and eigen function via iterative method by solving a set of equation at the boundaries. b and b þ L2. for which the wave functions extend in the forbidden regions outside the ADQW. multipliers of which form a determinant. > > > > > V2 > m2 . This determinant when equated to zero gives the allowed eigenstates.3d [5. the tight binding approximations and linear coupling of eigenstates have been used by many researchers [15–17]. we get a transcendental equation: ð sin k1 L1 þ pk1 cos k1 L1 ÞX þ ð cos k1 L1 À pk1 sin k1 L1 ÞY ¼ 0 ð3Þ .New XML Template (2006) {TANDF_FPP}TPHM/TPHM_A_181481. ¨ which are to be matched at four interfaces. Further complications are added when external boundaries of the wells are limited to the same height as of the barrier between the two wells (a case of great practical importance). A simple picture. Upon solving the determinant. Alternatively. This requires solution of Schrodinger’s equations in five different regions. 0. b x L2 > > > > > > : : 0 mb .2006–5:36pm] (TPHM) [1–11] [First Proof] 2 40 J. considers each of the two wells as having only one state and interaction between them is introduced as a perturbation [2]. enabling a clear understanding of the underlying physics. 12]. the most widely used of these being the Bastard’s envelop function method [13. 0 x b VðxÞ ¼ 0. R. These result in a set of eight equations for eight coefficients of integration.

7 6: þ2pk1 cos k1 L1 7 6 8 ÀðL þbÞ Â6 È 2 É 9 7. In the above equations. ' .2006–5:36pm] (TPHM) [1–11] [First Proof] Analytical expressions for an asymmetric double quantum well system 3 with X ¼ Àqk2 ðeb þ eÀb ÞðÀ cos k2 L2 þ qk2 sin k2 L2 Þ þ 2 ðeb À eÀb Þð sin k2 L2 þ qk2 cos k2 L2 Þ.6. 3m ðxÞ ¼ K 2pk1 þ eÀx ð2 þ p2 k2 Þ sin k1 L1 1 ð11Þ for b x L2: ¼K 1 2pk1 qk2 sin 2k2 b 3 28 9 È É > > eÀðL1 þbÞ ð À qk2 Þ ð2 þ p2 k2 Þ sin k1 L1 1 = < & 2 ' 7 6 2 2 sin k2 x 7 6 7 6 > þ eðL1 ÀbÞ ð þ qk2 Þ ð À p k1 Þ sin k1 L1 > . Y ¼ Àpk1 qk2 ðeb À eÀb ÞðÀ cos k2 L2 þ qk2 sin k2 L2 Þ þ pk1 ðeb þ eÀb Þð sin k2 L2 þ qk2 cos k2 L2 Þ 75 ð4Þ Since we are interested in eigenstate of ADQW.V2 < E < 0 so that the attenuation coefficient: pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi 2mb jEj ¼ h " ð5Þ ð6Þ 80 and the wave vectors pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi 2m1 ðE À V1 Þ 2m2 ðE À V2 Þ . : þ2pk1 cos k1 L1 4m ðxÞ ð12Þ . ð9Þ for –L1 x 0: 2m ðxÞ ¼ K eÀL1 pk1 & ð cos k1 L1 À pk1 sin k1 L1 Þ sin k1 x þ ð sin k1 L1 þ pk1 cos k1 L1 Þ cos k1 x ð10Þ 90 for 0 x b: " È É# eÀL1 ex ð2 À p2 k2 Þ sin k1 L1 þ 2pk1 cos pk1 L1 1 È É . 1 7 6 ð þ qk2 Þ ð þ p2 k2 Þ sin k1 L1 > >e 1 = < 7 6 & 2 ' 6 À 2 2 cos k2 x 7 ð À p k1 Þ sin k1 L1 5 4 > > þ eðL1 ÀbÞ ð À qk2 Þ .3d [5.New XML Template (2006) {TANDF_FPP}TPHM/TPHM_A_181481. we limit our solutions to V1 . k2 ¼ k1 ¼ h " h " ð7Þ are real. m1 and m2 are effective masses of electrons in the two wells and mb is that in the barrier regions and their ratios are denoted by: mb mb p¼ and q ¼ ð8Þ m1 m2 85 The corresponding wave functions are given by: for À15x ÀL1: 1m ðxÞ ¼ Kex .

7As) are plotted in figure 1 at different values of barrier width b. whatever the strength of coupling. When the barrier width is reduced.3Ga0. great interest has developed in potential wells formed in multi-layered semiconductor heterostructures. For such cases. The above equations are the most general and may be applied to any type of ADQW system. A large number of reports are available on effective mass and conduction band offset variations with respect to composition parameter x [23–27]. 0 x 0:45 1:0 ð14Þ 110 115 120 0:45 < x 125 130 The effective mass given above is conductivity effective mass. the probability density and energy eigenstates for ADQW structure with L1 ¼ 2. though the conclusions are of a general nature and can easily be extended to deeper wells with multiple states.3d [5. Using these parameters. We have taken the following dependences from [23]: mà ¼ 0:067 þ 0:083x & 1:1x. Contrary to this. Ram and S. Applications to semiconductor heterostructures (GaAs/AlxGa1–xAs) In the transcendental equation (3). shallow quantum wells with one or two energy states in each well are of practical interest [19. The basic difference between SDQW and ADQW is that the asymmetry results in localization in ADQW.6. As an illustration. for simplicity. belonging of eigenstates. We confine ourselves mainly to the study of these systems.3 (GaAs/Al0. In actual semiconductors. Furthermore. to individual wells and. charge distributions remain largely localized in individual wells. in present-day electronics. for larger separations.0 nm. R.2006–5:36pm] (TPHM) [1–11] [First Proof] 4 J. Here. For SDQW. we have taken constant effective masses for various regions.New XML Template (2006) {TANDF_FPP}TPHM/TPHM_A_181481. non¨ parabolicities may exist which will then make m* a function of E. the very fact of introducing asymmetry attaches. However. 22] and may be helpful in getting exact characteristics of the material. the effective masses will correspond to free electron mass and then p ¼ q ¼ 1.0 nm and x ¼ 0. Non-parabolicity of E – k relations will involve nonlinearities and exact solution of Schrodinger’s equation is not possible. However. the probability distribution extends . When the potential barriers are formed in vacuum. the scope of the present paper has been limited to assuming effective masses to be energy-independent. 3. we choose one of these systems as an example of application of the above equations. ÁEc ðxÞ ¼ 0:43 þ 0:14x. L2 ¼ 4. we have considered GaAs/AlxGa1–xAs heterostructure. the probability distribution is equal in both the quantum wells and a complete delocalization exists. 20]. This essentially assumes that E – k relations are parabolic. Dhariwal and for L2 x51: 5m ðxÞ ¼ 4m ðb þ L2 Þ eÀðxÀbÀL2 Þ ð13Þ 95 100 105 The constant K in the above equations is determined by normalization of the wave function for the entire space extending from À1 to 1. approximation methods are being used [21.

135 to the other well.1. (c) 0. mathematical formulae presented here are much simpler and easy to use.7As asymmetric double quantum well (ADQW) of QW widths L1 ¼ 2. so that the two QWs resonate. In these systems.3Ga0. Probability density in GaAs/Al0. The electron energy eigenstates obtained here using analytical formulae are similar in nature to those obtained by Ferreira and Bastard [3] using numerical methods. 140 145 ψψ ∗ ψψ ∗ ∗ . Such an alignment requires determination of exact well width of wider QW for a given narrow QW.3d [5.5 nm and in (d) energies of eigenstates are plotted against barrier width b.2006–5:36pm] (TPHM) [1–11] [First Proof] Analytical expressions for an asymmetric double quantum well system 5 ψψ Figure 1.5 nm.0 nm and L2 ¼ 4. (b) 1. for a finite coupling of QWs. is used to get lasing via inter-subband inverse population [4]. Transport optimization using variation in QW width Inter-well transition in ADQW heterostructure. the depopulated subband is aligned with the higher subband of the wider QW of appropriate size so that maximum transfer of electrons between the two becomes possible. However. It is generally believed that quick transfer of electrons in the system under consideration is due to minimization of energy difference.0 nm at different well separations: (a) 5 nm. we apply these analytical formulae to some cases of practical interest. Next. What we find here is that.6. 3. comprising of one narrow and one wide coupled QWs. such that difference in energy between eigenstates of the two isolated QWs is minimized. The mechanism that works in the process is shown in figure 2.New XML Template (2006) {TANDF_FPP}TPHM/TPHM_A_181481.

3d [5. The analytical formulae presented here can be used to calculate the exact width of the complementary QW. ψψ ∗ ∆ .2006–5:36pm] (TPHM) [1–11] [First Proof] 6 J. R. In these calculations.0 nm and b ¼ 1. whereas the dotted line in (d) shows an additional calculation for b ¼ 1.New XML Template (2006) {TANDF_FPP}TPHM/TPHM_A_181481. L1 ¼ 4. the probability of finding the electron in each QW become nearly equal. Probability density of the matched state is shared equally between the two coupled QWs as shown in (b) and the corresponding energies are shown in (d). which shows a minimum at the same value of L2 for which probability of finding the electron in the two QWs is equal. the higher the energy difference. Process of matched inter-well transfer of electron by varying the width of larger QW coupled to a narrower one is shown for an AlGaAs/Al0. energy for photon. for the eigenstate under consideration.7As ADQW system. 150 155 160 there always exists a finite energy difference between eigenstates. ÁE. as shown in figure 2b. which corresponds to minimum energy difference between nearest eigenstates in such a way that probability density of a particular eigenstate is shared equally between the two QWs. one shifts the system slowly from an asymmetric to a symmetric one in which.5 nm have been used in (a)–(c). It is this equalization of probability that makes the transfer efficient under an elastic tunnelling at the same energy rather than transfer of electron from one eigenstate to another. in which the inset gives the variation of difference of energy of the eigenstates ÁE ¼ E2 À E1. Ram and S.0 nm to depict the effect of increase in the strength of coupling. The stronger the coupling.6.3Ga0. As one tries to minimize ÁE by changing the width of QW. Dhariwal ψψ ∗ ψψ ∗ Figure 2. In addition.or phonon-assisted inter-well transfer of electron can also be calculated using these analytical formulae.

we note that size asymmetry in ADQW results in the preferential distribution of charge in the individual wells to which the particular states belong.0 nm. Variation of energy of the eigenstates with confining potential V2 is shown in (d) and inset shows the variation of difference of energy of the eigenstates of the two wells similar to that reported in the literature [11] for the ADQW system by applying an external electric field.3d [5.0 nm and L2 ¼ 4. The energy level separation at this point is similar to energy level splitting in SDQW. 165 170 ∆ . Furthermore. 3. Probability density in GaAs/Al0.3Ga0. An additional dotted line in (d) shows calculations for b ¼ 1. This confirms the proposition that the size asymmetry can be neutralized by introducing confining potential asymmetry in an opposite direction. As far as probability distribution is concerned.7As ADQW with QW sizes L1 ¼ 2. we find that. (b) 725 meV and (c) 850 meV are plotted. we note that the separation between the two eigenstates increases as one move away from the matched condition.2.3Ga0. by varying confining potentials V2 (or V1). Transport optimization using variation in confining potential The effect of variation of the confining potential by varying it for one of the wells.6. while keeping the other constant.7As ADQW of well widths L1 ¼ 2.2006–5:36pm] (TPHM) [1–11] [First Proof] Analytical expressions for an asymmetric double quantum well system 7 ψψ ψψ ∗ ψψ ∗ ∗ Figure 3. We note that the ground state of narrower QW reaches a minimum energy difference with respect to second eigenstate of the wider QW at V2 % 725 meV making the behaviour of ADQW system resembling a SDQW. QW separation b ¼ 2. is shown in figure 3 for a typically chosen GaAs/Al0.New XML Template (2006) {TANDF_FPP}TPHM/TPHM_A_181481.0 nm to depict the effect of increase in the strength of coupling.5nm and for confining potentials V1 ¼ 330 meV and V2 equal to (a) 550 meV. Here.0 nm. These show shift of charge density with variation of V2 and neutralization of size asymmetry for the given set of parameters for ground state at V2 ¼ 725 meV.0 nm and L2 ¼ 4.

0 nm. Dhariwal 180 185 the charge can be redistributed as shown in figure 3a and b. Conclusions Based on first principles. 210 . the electric field is equivalent to (V2 À V1)/b in the present formulations. separation of wells. In addition. Simply. such as individual quantum well widths and confining potentials.New XML Template (2006) {TANDF_FPP}TPHM/TPHM_A_181481. we have derived analytical expressions for an asymmetric double quantum well system. In addition. Transport optimization using variation in material composition 190 195 200 205 Results similar to those obtained by variation in V2 can also be obtained by variation in material composition of the alloy. we find that minimization of energy difference ÁE as well as probability redistribution can also be accomplished by suitably selecting the alloy composition. Thus.45Ga0. at this point. 4.2006–5:36pm] (TPHM) [1–11] [First Proof] 8 175 J. The effect of change in V2 with respect to V1 is equivalent to applying an electric field. The effect described above is similar to that obtained by applying an electric field. the size asymmetry can be compensated by varying the material mole fraction of the coupled QW. In figure 4. R. the probability of finding the electron in the two wells for the eigenstate under consideration is equal. since the purpose of an electric field is also to create a potential difference between the two wells. Here.0 nm and L2 ¼ 8. Thus. ADQW behaves like SDQW for this eigenstate. the estimation of Al mole fraction in the AlGaAs alloy itself is a very interesting problem and has been attempted rigorously by many researchers [26. As is clear from figure 4b and d. To elaborate. our calculations provide an easy means of calculating the effect of electric field on the eigenstates of ADQW. [11] by applying an electric field and.3d [5. and wave functions for corresponding eigenstates can be calculated using standard formulae provided by this method.55As/AlAs/AlxGa1–xAs system with size parameters L1 ¼ 4. in which a minima is obtained similar to that reported by Mourokh et al. In our calculation. there is provision to accommodate all necessary ADQW parameters. 28]. etc. A large body of evidences exists in the literature that the asymmetry of ADQW size can be neutralized by applying an external electric field [11. an effect similar to that obtained by varying QW width or confining potential. 3. 29]. in the inset of figure 3d. we have plotted energy eigenstates and probability functions for typically chosen Al0. effective masses in different regions.3.6. we have plotted the separation of energy levels ÁE ¼ E2 À E1 against V2. we provide simple and easy-to-use analytical formulae for calculating Al mole fraction by measuring the band offset data of the coupled heterostructure layer. This analytical approach provides the energy eigenvalues as roots of a simple transcendental equation. Ram and S. certain properties of these heterostructures depends on the Al mole fraction [30] and the mechanism underlying such effects can be better understood in terms of variation of energy states and probability redistribution in QWs using the analysis presented here.

(i) Effect of variation of separation of the two wells upon the energy eigenvalues and corresponding wave functions has been studied for an ADQW having one eigenstate for each isolated well. its experimental determination.45Ga0. The main feature of ADQW is localization of eigenstates in individual QWs compared to SDQW.6.5 nm.5 nm to depict the effect of increase in the strength of coupling. Results obtained are in agreement with those reported in the literature using numerical methods. in which a complete delocalization exists. whereas in (d) an additional dotted line shows calculations for b ¼ 1. we have discussed the applications of these analytical expressions for GaAs/AlxGa1–xAs semiconductor heterostructures.0 nm. This may help in understanding the properties arising due to variation in Al mole fraction and. as well as in understanding the underlying basic physics of ADQW. delocalization of probability density increases as a result of coupling when the barrier width is reduced. In ADQW. The effect is similar to that obtained by varying the confining potential of one of the QWs. Effect of variation of Al mole fraction in the Al0.3d [5. QW width parameters in (a)–(c) are L1 ¼ 4.55As/AlAs/AlxGa1–xAs system on the probability distribution and energy eigenstates. which reveal their simplicity in use and effectiveness in accommodating various material parameters.New XML Template (2006) {TANDF_FPP}TPHM/TPHM_A_181481. hence. (ii) The effect of asymmetry can be minimized for a particular eigenstate by varying the width of one of the QWs so that probability density 220 225 ∆ . L2 ¼ 8.2006–5:36pm] (TPHM) [1–11] [First Proof] Analytical expressions for an asymmetric double quantum well system 9 ψψ ψψ ∗ ψψ ∗ ∗ Figure 4.0 nm and b ¼ 2. 215 Furthermore.

Phys. Effects are similar to those obtained by applying an electric field and are in agreement with those reported in the literature. Ferreira and G. Stroscio. Rev. Defence Laboratory. Science 297 70 (2002). Prog. Baheti and the encouragement of colleagues. Director. [13] G. 44 229 (1987). Agullo-Lopez. [4] M. Appl. Carrascosa. K.H. V. Bhatnagar and G. IEEE J. B 24 5693 (1981). Thus. 7 710 (2001).C. Rev.R. [5] Y. Phy. M. [12] A. Horing. Lett. 62 173 (1990). Chen. 86 3822 (1999). M.K. Aguilar. Useful discussion with Professor B. G.. Jodhpur. Melloch. R. Brum and R. H. Rev. Phys. 75 1107 (1999). Ferreira. Domoto. Keyser. a simple mathematical formulation provides an important method for understanding. [15] D. Rev. Bastard. Manu Smrity. Hosoda. [11] L. Schumacher. [8] M. Kovalev and N. Les Ulis.G. T. Mourokh. Appl. et al. C. Lett. 92 176801 (2004). 1988). Solid State Phys. Appl. Bastard. Mod. Rev.6.W. Bastard.A. ¨ [10] R.2006–5:36pm] (TPHM) [1–11] [First Proof] 10 J. van der Wiel.M. Phys. [9] A. J. S. Mozume.3d [5. 255 260 265 . U. Phys.A.M.W. P. Kisin. Phys. [6] H.L. 250 References [1] G.F. Phys. Belenky. Mailhiot. Wave Mechanics Applied to Semiconductor Heterostructures (Les Editions de Physique. which in turn results in an efficient transfer of electrons. et al. Dhariwal 230 235 240 in two coupled QWs becomes nearly equal for that energy level. [3] R. J. L. 95 3557 (2004). Lett. Kolbas and N. Acknowledgement 245 The authors acknowledges the keen interest in the present work shown by Dr M. [2] W. P. M.. Rep. Phys. Mod. This occurs at the minimum energy difference between the eigenstate under consideration and its nearest state..M..New XML Template (2006) {TANDF_FPP}TPHM/TPHM_A_181481. D. Phys. Nisheet Saxena. Yoshida. Phys. Tripathi. 75 3258 (1999). De Franceschi. Appl. Am. Chang and M. Quantum Electron. 81 3870 (2002). 60 345 (1997). U. Elzerman. F. [7] J. investigating and optimization the properties of ADQW.. 52 431 (1984). Bhandari. Huttel. J. which in turn can be calculated using the analytical formulae presented here. Bastard. Neogi.M. Dinesh and Jagdish. (iv) The consequences of varying Al mole fraction on the properties of these heterostructures and estimation of the Al mole fraction itself is of great practical interest and can be better understood in terms of band alignment and probability redistribution. corresponding to minimization of asymmetry and ADQW behaving like a SDQW for this state. A. J. et al. Zeitler. Phys. A. et al. et al. U. G.. et al.M. (iii) The biasing of ADQW result in interesting properties and its variation can be used in tuning the QWs in a way similar to that obtained by varying QW width. are gratefully acknowledged. S. [14] G.G. Holleitner. Appl. R. Blick. Lett. Hirose. B 25 7584 (1982). Holonyak Jr. K..J. Phys. Ram and S. 75 1 (2003). Bastard. Smith and C. Chacharkar. et al. Mirdha. J. S.

Nag and S.R. Phys. D.. Potemski.F. DiMaria. 87 2956 (2000). Phys. 93 186802 (2004). Wright. P. M. Wasilewski. S. S.H. Mashita. Phys..B. B. Batey and S. J. Lett. Mukhopadhyay. Johnson. Pescetelli. ¨ B. 74 2002 (1999).K. R. Ludwig. Duke. Phys. Lett. Yoshida. A. et al. J. Holleitner. S.R. 152 683 (1966). Phys.. 59 200 (1986). 57 484 (1985). Lockwood.W.J.. J. Phys.L. Petta. Nag and S. Bernardini. Paciotti. Phys. Rev. 11 270 275 280 .. Phys. D.New XML Template (2006) {TANDF_FPP}TPHM/TPHM_A_181481. J. et al. cond-mat/0501012 (2006). Watanabe... 58 R1 (1985). et al.2006–5:36pm] (TPHM) [1–11] [First Proof] Analytical expressions for an asymmetric double quantum well system [16] [17] [18] [19] [20] [21] [22] [23] [24] [25] [26] [27] [28] [29] [30] F. 62 2416 (1993). Di Carlo.J. Status Solidi (b) 175 103 (1993). M. Huttel. C. T. Wolford.M. 51 505 (1987).L.H. Appl. F.J. Appl. Phys. J. Phys. Lett. Ben Daniel and C. Batey. 81 1683 (1997). J.R. 57 5340 (1985). J. A. Phys. Appl.C. A. Wright and D. Appl. S. A. Dion. M. K. Blick.R.M. Huttel. Eberl. Della Sala. Appl. Lugli. Science 297 70 (2002). ¨ Z. Lett. A.C. Kuech. Phys. J. Appl. Marcus. J. Mukhopadhyay.. et al.O. 98 803 (1996). et al. Appl. Appl. Appl.6. Adachi.J. R. M. Solid State Commun. et al. et al.3d [5. Choy.K. Rev. W. D. J. et al.

Though.com/locate/physb Suppression of nonradiative recombination in small size semiconductors S.67.13].033 . E-mail address: dhariwalsr@yahoo. accepted 20 February 2005 Abstract Enhanced optical efficiency of nanosized semiconductors is due to reduction in the nonradiative recombination rate.6.20. This explains the reduction of nonradiative recombination in small size grains. fax: +91 291 2510260. Nonradiative.V.20.8] and much work has been done on optical transitions and spectral analysis [3.02. Dhariwal). Dhariwala.Jv. doi:10.2005. due to it’s indirect band gap was never considered useful material for light emitting devices until the discovery of porous ÃCorresponding author. Jasa Ramb a Department of Physics. Optical efficiency. All rights reserved.1016/j.9–11]. We show in this paper by a first-order theory that small grain 0921-4526/$ . 78.5. Particularly silicon.Ã. received in revised form 19 February 2005. 78. r 2005 Elsevier B.15].V. India b Defence Laboratory.see front matter r 2005 Elsevier B.ARTICLE IN PRESS Physica B 363 (2005) 69–75 www.6] and increased oscillator strength [7. Jodhpur 342 001. The nonradiative processes compete with radiative ones and it is their relative magnitude that decides the efficiency of light emission [14. PACS: 72. little attention has been given to nonradiative recombination processes [12. Recombination.68.R. silicon in which due to quantum confinement light emission of practical use could be obtained [1–4].Bh.R. Introduction Nanocrystalline and microcrystalline semiconductors have found wide applications in optoelectronic devices because of their increased optical emission efficiencies compared to bulk materials [1–3]. A theoretical basis for such a reduction is obtained by a classical approach by calculating surface recombination velocity in a confined configuration. All rights reserved. it has been well established that an increased optical efficiency of nano-sized semiconductors as compared to bulk material is due to quantum confinement [2.Àn.elsevier. Nanostructures 1. Jodhpur 342 011.+m Keywords: Semiconductors. Tel.com (S. as the size of the grain is decreased.physb.: +91 291 2722543. 78. India Received 18 January 2005. Jai Narain Vyas University.

ARTICLE IN PRESS 70 S. so that df ¼ nvR dS which gives ZZZ Àr=l  e cos y vR ¼ vth dV . The capture event can be described as follows: Free electrons (or free holes) are scattered continuously in all directions due to the various collision processes in the semiconductor. dV = r 2 sinθ drdθdϕ r θ dS Fig. the flux of electrons directed from volume element dV to surface element dS is dS cos y n dV . we analyse the effect of finite grain size on surface recombination velocity. the probability of electrons starting from dV to reach dS uninterrupted is eÀr=l : Thus. Quantum mechanical effects [16] arising in the charge transport due to size reduction have been neglected in this firstorder theory. However. 1. 1. Calculation of surface recombination velocity Nonradiative recombination usually proceeds via a localized trap [17]. (4) eÀr=l df ¼ vth 4pr2 l Let us now define by vR the average of the normal component of the velocity with which electrons of density n are reaching the surface element dS. The model presented here is based on the assumption that effective mass approximation remains valid for smaller size grains and is invariant under size reduction. l 4pr2 (5) (6) . As the size of the grain reduces. Of these. the flux of the electrons reaching the surface element dS from volume element dV is eÀr=l dS cos y n dV . Thus. the electrons which are directed towards a surface element can be captured provided they do not meet a second collision in the path. For this reason. 4pr2 t (2) This when integrated over the entire volume of the semiconductor gives the flux of the electron reaching the surface element dS. enhances the radiative processes. as the size is decreased. we evaluate the effect of finite size of the surrounding medium (semiconductor) on the rate of recombination. if l is the mean free path of the electrons. the surface to volume ratio increases and recombination is more likely to occur at the surface rather than the bulk. A free electron moving in the surrounding space is captured by an empty trap (nonradiative recombination centre) which can subsequently capture a free hole. The solid angle subtended by the surface element dS on the volume element dV is dS cos y=r2 for configuration shown in Fig. which has been assumed to be uniform and t is the mean collision time. J. a scattering centre in a volume sends electrons in all directions. Dhariwal. similar conclusions can be drawn for bulk lifetime. If n is the density of electrons in the bulk semiconductor. This leads to enhanced optical efficiency in micro and nanosized semiconductors. 2. 4pr2 t (1) Further.R. (3) df ¼ e 4pr2 t If vth is the average thermal velocity of electrons then l ¼ vth t and we have ZZZ  cos y n dV dS. A surface element dS in a semiconductor of semi-infinite geometry. ZZZ  Àr=l cos y n dV dS. In this paper. Ram / Physica B 363 (2005) 69–75 size suppresses the nonradiative recombination and hence.

J. . r tan d ϕ W cos α r θ (a) dS (b) r= W θ dS r tan θ Fig. Semi-conductor slab of finite thickness Now.2. contribution of bulk in the flux of electrons reaching dS. Semi-infinite geometry Let us now calculate vR for a semi-infinite geometry. we introduce confinement in the problem. 2. pr2 Here cos a is the direction cosine of the surface element dA with respect to vector ~: The flux r received by the element dS from the entire surface is obtained by integrating the above expression on the surface element dA and it is given by ZZ cos y cos a dS dfS ¼ n eÀr=l dA: (13) pr2 For an element dA on a plane surface at a distance dA dA = r dθ . it will reflect (re-emit) a fraction of the electron flux incident on it. Z p=2 Z W = cos y Z 2p Àr=l e cos y vW ¼ vth R l 4pr2 y¼0 r¼0 j¼0 Â r2 sin y dy dj dr.2. However. Configurations for capture at surface element dS (a) from a general surface element dA and (b) for a slab of thickness W. vth . For pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi a non-degenerate electron gas ffi vth ¼ 8KT=pm pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi and therefore v1 ¼ KT=2pm which has the R same meaning as used in thermionic emission theory [18].R. B R R (12) Thus. If this surface is not completely absorbing. 2.1. For this case the limits of integration on r for a given y will be from 0 to W = cos y: This gives.ARTICLE IN PRESS S. For this case. the confinement itself is due to the presence of another surface at a perpendicular distance W from the element dS.1. Ram / Physica B 363 (2005) 69–75 71 2. we have Z 1 Z p=2 Z 2p Àr=l e cos y 2 1 r sin y dy dj dr vR ¼ vth l 4pr2 r¼0 y¼0 j¼0 (7) which upon calculating integrals gives. dfW ¼ nvW dS ¼ bnv1 dS. 2. Dhariwal. If n is the emissivity of the surface then flux of the electrons reaching dS from dA for a diffused emission is given by n eÀr=l cos y cos a dS dA. For this let us consider a semiconducting slab with electrons confined between surfaces at z ¼ 0 and W. ð9Þ On solving the integral on r and j and by letting cos y ¼ x we get vW ¼ bv1 R R (10) with   W x exp À dx b¼1À2 lx x¼0 Z 1 (11) and therefore. (8) v1 ¼ R 4 where v1 is the average of normal component of R velocity with which electrons are received at the surface element dS in a semi-infinite geometry. the effect of space confinement is to reduce the contribution of bulk semiconductors in the flux of electrons reaching the surface element. Contribution from surface To calculate the contribution of the surface let us consider a surface element dA as shown in Fig. 2.

j). (16) we get. W reduces and dfW starts increasing. dfW ¼ ð1 À f a Þð1 À bÞnvR dS. the rate of recombination at the surface element dS However.2. it will be zero. However. As confinement S increases. dfW ¼ ð1 À bÞn dS. if we neglect inter-granular transport. (5). Dhariwal. nvR dS ¼ nbv1 dS þ ð1 À f a Þð1 À bÞnvR dS. It is the absorptivity of the surface introduced for confinement that limits the flux reaching the surface element dS and reduces the value of vR. However. in which it is first absorbed in excited state and then falls to ground state. we note that the total flux reaching the surface is df ¼ dfB þ dfS . The actual value of fa will vary between 0 and 1.ARTICLE IN PRESS 72 S. the capture in deep states is through a cascade process. surface acts as a secondary source of electrons. we have dA ¼ W dy W tan y dj. for a highly disordered surface. If Nti is density of the surface recombination centers of capture cross-section si then for P low density of the traps f a % i N ti si : However. S Now. isolation of the traps assumed in the above summation may not be valid and one has to assume an effective value of fa which will always be less than unity. Thus. W ! 1 and dfW is zero. S (16) We note that depending on emissivity. ½vR Šf a !0 ¼ v1 ¼ vth =4: This is a statement of R conservation of charge and proves the consistency of the calculations. The charge conservation may require a third term ft for transport of carriers from one grain to another. (12) and (20) we get. cos2 y (14) 1 À f a and therefore. For a semi-infinite geometry. For this. as explained by Lax [19].2. we have f a þ f r þ f t ¼ 1. Surface recombination velocity If SR is the surface recombination velocity. For an completely absorbing surface fa is unity whereas for a completely reflecting surface with no recombination centers on it. the surface element dA may reflect back the carriers due to surface barriers. ft can be assumed to negligible and we have f r ¼ . Ram / Physica B 363 (2005) 69–75 W.  Z 1    W dfW ¼ n 2 x exp À dx dS (15) S lx 0 which gives. Thus. (18) The rate of recombination at the surface in terms of sticking probability is given by dR ¼ f a df. with angular positions (y. a large portion of the surface may have shallow traps at which electrons are captured and are re-emitted very effectively. Also. By using Eqs. integrating we get. we note that a surface has a large number of deep as well as shallow traps. (13) and by noting that for the geometry under consideration a and y are equal. 2. the contribution from surface is complementary to that from bulk. fa is different for different types of traps present on the surface. Further. n ¼ f r nvr ¼ ð1 À f a ÞnvR . (19) Upon putting this value of dA in Eq. (17) The sticking probability fa for the surface denotes the capability of the surface element to absorb the electron.R. R so that vR ¼ b v1 . we can define by fa the probability of the electron sticking to the surface. for a perfectly re-emitting surface. they will capture electrons and may hold them for sufficient time to allow the subsequent capture of holes so that recombination takes place. The deep traps are the recombination centers and if these are empty. Thus. it remains for us to relate emissivity of the surface with the flux incident on it. 1 À ð1 À f a Þð1 À bÞ R (23) (22) (21) The above equation shows that confinement reduces vR through absorptivity of the surface fa. J. On substituting the value of n in Eq. S (20) Now. All these processes can be lumped together in terms of reflection coefficient fr which is assumed to be arising mostly due to diffused reflectance/re-emission.

wherein the normal to dS makes an angle (p=2 À j) with the r–z plane. (5) and (19) give S R ¼ f a vR . Ram / Physica B 363 (2005) 69–75 73 can be written as. Eq. Z 1 Z p Z D sin j Àr=l e cos y sin j vD ¼ vth R 4pr2 l z¼À1 j¼0 r¼0  r dj dr dz. 3. (29) 2 þ r2 z which can be further simplified to give  À1 1 1 S R ¼ v1 þ À1 . Thus. R fa b (27) Thus. (16)–(27) are based on the basic principle of space confinement and therefore. (27) can be applied to other geometries also provided the weight factor b for the flux coming from the bulk is known. Dhariwal.ARTICLE IN PRESS S. we note that the contribution arising from emissions from the surface is complementary to that from the bulk. Reduction in either fa or b reduces the value of SR. For a grain of diameter D. (27) to other geometries. 4. This by using equating Eqs. In terms of v1 the surface recombination velocity R becomes SR ¼ f ab v1 1 À ð1 À f a Þð1 À bÞ R (26) (24) 2. The surface element is located at the origin of the cylindrical coordinate system.3. Cylindrical grain From Eq. we derive the expression for b using cylindrical geometry shown in Fig. we find that. As an attempt to extrapolate Eq. pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi r r ¼ z2 þ r2 and cos y pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi . Such a situation may typically arise in semiconductor wires like those in porous silicon. apply to all types of configurations. we note from above expression that surface recombination velocity SR is highest for a semi-infinite system with perfectly absorbing surface and it’s value is given by v1 ð¼ vth =4Þ: This is R the velocity with which an infinite sink will absorb the particles arriving at it. . z ρ dS 90° r θ dV = ρ dρdϕdz D ρ ϕ dS z (a) (b) Fig. whereas reduction in b will arise if the space provided for electrons to move is reduced from semi-infinite to a finite geometry. Eqs. 3. The reduction in fa is due to re-emission from the surface. dR ¼ S R n dS. ð28Þ The factor sin j in above equation arises due to the cylindrical geometry considered here.R. Irrespective of the geometry. (a) Configuration for a trap at the surface of cylindrical semiconductor column and (b) cross-sectional view of this configuration. J. The above equation clearly brings out the effect of confinement on surface recombination velocity. From the geometry shown in Fig. the surface recombination velocity is product of the velocity vR with which the electrons reach the surface and their sticking probability fa. (25) Thus. (16).

4 0.8 ∞ SR /vR The surface recombination velocity SR for this case can be calculated by replacing b by b1 in Eq.4 0.1 3.9 fa = 0.. Similar expressions can be obtained with somewhat more involved geometry for quantum dots with basic conclusions remaining the same..7 fa = 0. 77K fa = 1. We may point out here that in our calculations. Surface recombination velocity SR as given by Eq. 77K fa = 1.5 fa = 0. we use typical values for silicon. (27). As is clear from the diagram. (27) for a semiconductor slab for different values of sticking probability fa is plotted against thickness W of the slab for silicon at temperatures 300 and 77 K.R. (31).0 fa = 0. the conclusions are of general nature and will apply to bulk traps as well. Thus. 5. the surface recombination velocity reduces with decrease in grain size and a much more pronounced effect is observed at lower temperatures.1 10-8 D (m) 10-7 which upon putting values of constants for silicon give l¼ 1:4 Â 10À5 m. 4 as a function of thickness W for some typical values of sticking probability fa at 300 and 77 K.2 fa = 0. 5 shows values of SR for a cylindrical grain calculated by using Eq. we have assumed a constant capture cross-section.0 0. v D ¼ b1 v 1 R R with 4 b1 ¼ p Z 1 z¼0 (30) Z Z pffiffiffiffiffiffiffiffiffi À 2 2 l p=2 D sin j e z þr =l r sin j fz2 þ r2 g3=2 ð31Þ j¼0 r¼0 Â r dj dr dz.0 fa = 0.1 Fig. (27) are plotted in Fig.3 (32) 0. The values of surface recombination velocity SR for a semiconductor slab given by Eq. Dhariwal. Ram / Physica B 363 (2005) 69–75 1. we obtain. T (33) Fig.9 fa = 1. 1. Surface recombination velocity SR as given by Eq. On substituting these values.3 fa = 0. Also. (31) for silicon at 300 and 77 K.5 fa = 0. though we have confined our calculations to surfaces.0 10-9 fa = 0. J.9 fa = 0. .0 10-8 W (m) 10-7 _____ 300K …. For a semiconductor cylindrical column. In actual situation. (27) with b replaced by b1 as given by Eq. 4..ARTICLE IN PRESS 74 S. the decrease in the size of grain reduces the capture rate from the bulk and the effect is more pronounced at lower temperature. Results presented here are for silicon at 77 and 300 K for different values of fa.7 0. We assume a deformation potential scattering dependent mean free path given by [20] l¼ p_ cl m 2 2 k BT 4 0.8 0. Discussion and conclusions To illustrate the effect of confinement.6 0. In the case of cylindrical grain also. This applies both to the semiconductor quantum wires like those in porous silicon and semiconductor slabs in superlattices.. (27) is plotted against diameter of cylinder D using b1 as given by Eq.7 fa = 0.0 0. ∞ SR /vR ____ 300K …….6 fa = 0.5 fa = 0. reduction in the size of the semiconductor has a direct bearing on the efficiency of light emitters which show better performance when reduced to nanoparticle size.0 fa = 0.3 fa = 0.2 0. Fig..

ARTICLE IN PRESS
S.R. Dhariwal, J. Ram / Physica B 363 (2005) 69–75 75

the traps have many excited states and recombination is usually through a cascade process [19]. As the size of the semiconductor is reduced to quantum size, these excited states may disappear and may result in drastic reduction in capture cross-section. This will further reduce the nonradiative recombination making these semiconductors more efficient emitters of light. In this paper, we have brought out the effects which have to be incorporated in the Shockley Read Hall model of recombination, if one wants to use it for small size grains. Quantum confinement may give rise to additional factors which have not been included here.

Acknowledgement One of the authors (J.R.) acknowledges with thanks keen interest in this work shown by R.K. Syal, Director, Defence Laboratory, Jodhpur. References
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[3] A. Malini, S. Novikov, V. Ovchinnikov, V. Sokolov, O. Kilpela, T. Saloniemi, J. Sinkkonen, Light emission from silicon-based materials, Report in Electron Physics 2001/ 25. [4] L.T. Canham, Appl. Phys. Lett. 57 (1990) 1046. [5] G.M. Credo, M.D. Mason, S.K. Buratto, Appl. Phys. Lett. 74 (1999) 1978. [6] D.P. Yu, Z.G. Bai, J.J. Wang, Y.H. Zou, W. Qian, J.S. Fu, A.H. Zhang, Y. Ding, G.C. Xiong, L.P. You, J. Xu, S.Q. Feng, Phys. Rev. B 59 (1999) R2498. [7] V. Ranjan, V.A. Singh, G.C. John, Phys. Rev. B 58 (1998) 1158. [8] P.F. Trwoga, A.J. Kenyon, C.W. Pitt, J. Appl. Phys. 83 (1998) 3789. [9] A.G. Cullis, L.T. Canham, P.D.J. Calcott, J. Appl. Phys. 82 (1997) 909. [10] M.S. Hybertsen, Phys. Rev. Lett. 72 (1994) 1514. [11] M.V. Rama Krishna, R.A. Friesner, Phys. Rev. Lett. 67 (1991) 629. [12] J.C. Vial, et al., Phys. Rev. B 45 (1992) 14171. [13] G.W. ‘t Hooft, Y.A.R.R. Kessener, G.L.J.A. Rikken, A.H.J. Venhuizen, Appl. Phys. Lett. 61 (1992) 2344. [14] R.M. Mehra, V. Agarwal, V.A. Singh, P.C. Mathur, J. Appl. Phys. 83 (1998) 2235. [15] G.C. John, V.A. Singh, Phys. Rev. B 54 (1996) 4416. [16] C. Delerue, et al., Phys. Rev. B 48 (1993) 11024. [17] W. Shockley, W.T. Read, Phys. Rev. 87 (1952) 835. [18] S.M. Sze, Physics of Semiconductor Devices, Wiley, New York, 1981, p. 261. [19] M. Lax, Phys. Rev. 119 (1960) 1502. [20] K. Seeger, Semiconductor Physics—An Introduction, third ed., Springer, Berlin, 1985, p. 167.

TRANSPORT AND RECOMBINATION MECHANISMS IN NANOCRYSTALLINE SEMICONDUCTORS
ABSTRACT OF THESIS SUBMITTED FOR THE DEGREE OF DOCTOR OF PHILOSOPHY (PHYSICS) BY

JASA RAM

under the supervision of

Prof. S.R. DHARIWAL

DEPARTMENT OF PHYSICS, JAI NARAIN VYAS UNIVERSITY JODHPUR – 342 005 INDIA July 2006

ABSTRACT: Transport And Recombination Mechanisms In Nanocrystalline Semiconductors

ABSTRACT
Quantum confinement has re-defined the science in many streams [1], particularly in semiconductors many new phenomena seem to emerge at this scale. In recent times, most noteworthy consequences of quantum confinement have been reported on the transport and recombination properties in nanosized semiconductors [2-5] which has put on demand for quantitative understanding of mechanism responsible for such novel phenomenon and applications. Since, quantum well (QW) is a basic unit for investigation of quantum confinement associated effects, the consequences of coupling upon eigenstates of coupled QWs [4, 6] and actual interplay between eigenstates of coupled QWs with charging of individual QWs [2-4, 7] forms the studies of major practical interest [8, 9] and enable the quantitative description of electron transport in nanosized semiconductors. Also, eigenstates of coupled QWs largely determine the designing of quantum point contacts (QPC) [10] for transport of electron through a quantum dot (QD). As far as the transport of electron through a QD is concerned [11], the recently reported anomalous universal phase evolution in coherent transport [12, 13] has attracted much of attention, satisfactory explanation of which is not available [12, 14] so far and is a much sought

-1-

16] and little attention has been at nonradiative recombinations [17]. In this area. 15. enhancement of radiative recombination has been a subject of wider study [5. In this chapter. 15. 16]. The field is blossoming and there is a great spreading out in the novel application of new and exciting phenomenon reported in recent times. applications of charge transfer between QWs. namely: determination of eigenstates of coupled quantum wells. localization and delocalization positions and their sequences as -2- . perturbation of eigenstates. the recombination mechanisms have been a subject of wide investigation in accounting for the enhanced optical efficiency in nanosized structures [5. The present thesis aims to pursue quantitative understanding of the sciences of transport and recombination in this new class of materials and structures. the survey of literature has been divided in various parts. after an overview. A brief account of the work carrier out and conclusions arrived at is being discussed chapter wise in the following paragraphs. a review of literature in the field of transport and recombination in nanosized semiconductors in perspective of the preset work has been given along with outline of the proposed work. In the Chapter 1.ABSTRACT: Transport And Recombination Mechanisms In Nanocrystalline Semiconductors after problem. charging of QWs and QDs. The thesis is comprised of seven chapters. In addition to quantum confinement.

ABSTRACT: Transport And Recombination Mechanisms In Nanocrystalline Semiconductors well as significance. localization is decreased for strong coupling strengths. and radiative and nonradiative recombination mechanisms in nanosized semiconductors. All ADQW parameters such as QW widths. corresponding to minimization of -3- . This occurs at the minimum energy difference between the eigenstate under consideration and its nearest state. First principle based analytical expressions have been derived for determination of eigenstates of coupled QWs modeled as asymmetric double quantum well (ADQW) system in the Chapter 2. Using these formulae. However. transport through a QD and universal phase evolution. effective masses jumps etc have been accommodated in the formulation. It is shown that the effect of asymmetry can be minimized for a particular eigenstate by varying QW width and / or confining potential so that probability density in two coupled QWs becomes nearly equal for that energy level which in turn results in an efficient transfer of electrons. Some of the applications of these analytical formulae have been discussed for GaAs / AlXGa1-XAs semiconductor heterostructures. missing in symmetric double quantum well (SDQW). it is found that the strong localization behavior of the eigenstates of the individual QW is clearly a feature of ADQW. QW separation. The literature survey clearly brings out the necessity of quantitative understanding of transport and recombination phenomena. confining potentials.

Further. transfer of electron between coupled QWs at zero perturbation position has been discussed in view of its possible applications. -4- . The universality of this zero perturbation position has been proved graphically as well as analytically and its explanation has been given in terms of transmission line theory. it is shown that variation in alloy composition can also be used for transport optimization between QWs. While investigating the effect of strength of coupling upon eigenstates of coupled QWs using the analytical expression for ADQW derived in Chapter 2. The effect of varying confining potential for transport optimization is shown to be identical to that obtained by applying an electric field.ABSTRACT: Transport And Recombination Mechanisms In Nanocrystalline Semiconductors asymmetry so that ADQW behaves like a SDQW for this state. the detailed analysis of which has been presented in the Chapter 3. This position corresponds to phase in integral multiple of π traveled by an electron wave through the coupled QW. Further. it is found that for every QW for a given eigenstate another QW can always be found which is completely matched with the host irrespective of coupling strength and electron can tunnel from the host to the guest without perturbing the former.

The sequence and significance of charge transfer positions between QWs and the change of eigenstates of interest have been analyzed and the effect of coupling strength as well as asymmetry on these has also been presented. This study is aimed at understanding the mechanism of electron transfer between QWs and QDs.ABSTRACT: Transport And Recombination Mechanisms In Nanocrystalline Semiconductors Further to applications of analytical expressions for ADQW discussed in Chapter 2. The efficacy of the analytical expressions for ADQW system derived in the Chapter 2 in respect of the applications discussed therein and the phenomena presented in the Chapter 3 and 4 clearly reveal their simplicity in -5- . the entire spectrum of energy eigenstate gives an appearance of staircase type of picture in which each state goes down by one step around the crossover at which the occupation probability sharply changes their belonging from first QW to second QW and thus giving rise to a resonant effect. The process of electron transfer involves one energy state being replaced by another of opposite parity and coupling changes alternatively between symmetric and anti-symmetric one. Next. These charge transfer studies may form the basis of various applications of coupled QWs. the interplay of eigenstates of ADQW system and the charge transfer between QWs has been investigated in the Chapter 4 by determining the fractional occupancies of electron in the two QWs. each resonance corresponds to an electron transfer and the spectrum going down by one step.

In Chapter 5. a QD acts as an artificial tunnel which is neither open nor closed and therefore. expression for coherent component of the transmission coefficient for QD modeled as double barrier quantum well system has been derived by separating the directly coupled component from those due to multiple reflections in the conventionally obtained transmission coefficient which in turn has been derived in terms of the QW coupling coefficients. little attention has been paid to the study of reduced size on the -6- . We find that directly transmitting component gives the coherent transmission coefficient and magnitude and phase of this coherent component is in agreement with the universal phase evolution in electron transmission through a QD and thus provide an explanation of the much sought after problem. However. the efficiency of these devices depends on the relative magnitudes of radiative and nonradiative recombination rates. For transport studies.ABSTRACT: Transport And Recombination Mechanisms In Nanocrystalline Semiconductors use and effectiveness in accommodating various material parameters as well as in understanding the underlying basic physics of coupled QWs and QDs. it is a fascinating problem to study where the role of quasi bound states of the QD is also crucial. Increased radiative recombinations have been a subject of wide investigation in accounting for the enhanced optical efficiency in nanosized semiconductors. In fact.

surface recombination velocity is shown to be reducing as the size of confining structure is decreased. simplified expressions for surface recombination velocity for electrons confined between parallel plates resembling heterostructures and in cylindrical grains resembling quantum wires have been derived which are based on the first principle semi-classical calculations. Using these expressions. enhancement of optical efficiency in nanosized structures. The summary of the work carrier out and gist of the conclusions drawn have been included in the Chapter 7. In Chapter 6. -7- . This proves the suppression of nonradiative recombination and hence.ABSTRACT: Transport And Recombination Mechanisms In Nanocrystalline Semiconductors nonradiative recombinations. The conclusions are of general nature and apply to nanosized cluster of any shape.

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