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**MULTIPLE EXCITON GENERATION IN QUANTUM DOTS
**

Oksengendler B.L., Turaeva N.N., Rashidova S.S.

Institute of Polymer Chemistry and Physics, Uzbekistan Academy of Sciences,

100128 Tashkent, Kadiriy street, 7B, Uzbekistan.

E-mail: nturaeva@hotmail.com

Abstract

The statistical theory of multiple exciton generation in quantum dots which is based on

the Fermi approach to the problem of multiple particle in nucleon-nucleon collisions is

presented. Our estimates of the multiple exciton generation efficiency in different quantum dots,

induced by absorption of a single photon, are in a good agreement with the experimental data.

**Carrier multiplication (CM) phenomenon in confined nanostructures was predicted by
**

A.Nozik of NREL in 2002 [1]. In 2004, Klimov and co-authors reported that PbSe nanocrystals

can respond to absorption of a single photon by producing two electron-hole pairs with 200%

efficiency. This carrier multiplication phenomenon, also known as multiple exciton generation

(MEG) [2]. Later the effect of MEG has been experimentally confirmed by NREL team [3] by

investigating PbSe and PbS quantum dots of 3 different sizes in which increasing of quantum

yield up to 300% has been observed. Recently it was revealed by Schaller et al. [4] that MEG is

the real phenomenon with generation to up 7 excitons in PbSe QDs (Еg=0.3 eV and R=20 nm) at

absorption of a single photon with energy of h=7.8 Еg.

Using carrier multiplication Klimov [4,5] has demonstrated ―exotic‖ non-Poissonian

distributions of carrier populations. Different groups have reported recently the formation of

multiple excitons based on the femtosecond transient spectroscopic observations. Possible

applications of the effect in constructions of on Polymer-QD based solar cells [6] and for low

threshold laser design [7,8].

It should be noted that besides practical applications the MEG effect can be used as a

testing ground for new kind of nonlinear photo effect. The theoretical analysis of MEG related to

two or three excitons generation has been considered in several studies by Schaller R.D. et al.

[9] and Elingson et al. [3]. Despite the considerable amount of papers on MEG the problem of

theoretical explanation of MEG of higher multiplicity in QDs still remains open. In our opinion,

this is caused by the fact that the application of perturbation theory to the charge multiplication

effect (e.g. as used in [9]) is complicated for the processes of higher multiplicity. Recently some

other approaches to theoretical understanding the mechanism of MEG have been considered (see

[9,10]). However the final conclusion is that the mechanism of MEG is not fully revealed yet.

S n n . R is the radius of QD and the number of particles is even number: n= 2. Then it can be shown that the probability for n-particles 2 generation in the volume of is proportional to the statistic weight: 3n S n m 3n / 2 n 2 3n / 2 3n / 2 3n n ~ 2 h E g 2 3n 1! 2 1 .10. we suppose that in the case of multiple excitons generation the high energy photon is absorbed by a QD and according to statistic laws the absorbed energy is quickly distributed among the various degrees of freedom.8.14. Namely.78 e 2 ~ Here m is the electron mass. Here we take into account the fact that the total kinetic energy is defined by the difference of photon energy and energy gap multiplied by the n number of excitons T h E g . In this paper we present a mechanism of MEG in QDs which can be treated using the combination of statistical theory and on Fermi approach [11] to the multiple particle creation inhigh-energy nucleon-nucleon collisions.4. In this case using the Fermi`s formula we can calculate the probability for n-particles generation with a given energy distribution in a small volume of QD.6. The latter was originally used for the analysis of the generation of elementary particles – nucleons and mesons in high-energy nucleon-nucleon collisions.12. E g E g [14]. in which the second term describes the R electron-hole interaction energy.Therefore other mechanisms need to be considered for explaining the highest MEG efficiencies. Unlike the perturbation theory used in [9]. and namely this factor sharply increases the probability of statistic equilibrium setting. In addition. this approach is based on the strong interaction of correlated electrons with electromagnetic field in a QD. in a QD of volume n/2 excitons are generated where n is the total number of produced particles (electrons and holes). In particular. Then the relative probability for n-particles generation is given by the following expression: W ( n) S n . 1. the above mentioned non-Poissonian character of exciton multiplicity which has been recently experimentally observed [5] needs also to be explained from the in theoretical viewpoint. We argue that the Fermi theory seems to be closer to the reality in a high energy range when the number of possible exciton states with given energy is large.

. For Si QDs (Еg=1. For example. n 2 187. [5]. h=3. For the case of PbSe QDs (Еg=0. I n1 is the overlapping integral of n1 electrons wave functions in valence and conductive zones of QD. Such effect is studied in detail by several authors (see.4Еg) we have theory N exc 2. observed experimentally in the Ref. where the average number of excitons in QD N exc is calculated using on the following equation: n 2 N exc nS n .64eV. h=3.e. reviews [12] and references therein)Using the same approach as that for the calculation of multiple ionization of atoms by its shaking in the collisions with fast ions. e.1 . in the case of PbSe QD (R=20nm. For PbSe QDs (Еg=0.8Еg) we can show that n 13. It means that the condition for Poissonian distribution is not valid for the effect of MEG as it was shown in [5].7 . h=7. i.84 and N exc [9]. we suppose that the microscopic mechanism of the effect is connected to the shaking effect of several electrons caused by the primary exciton at absorption of high energy photon.5 nm. For PbSe QDs (Еg=0.00 ) [9]. Here 1ex is the cross-section of primary exciton generation. Furthermore.25 [9]. R=3. h=7. R=20nm.The quantum efficiency of multiple excitons generation by a single photon can be written as QE 100% N exc .9nm. h=4. the cross section for generation of n electron-hole pairs induced by one-photon-absorption: a R n 1ex I n21 .3eV.2 [10].9Еg) we have theory N exc 2.62 and exp N exc 2. 2. exp theory 3. we can estimate the MEG cross section.63Еg) we have N exc 2.2eV.64eV.0 6. 4. R=9.85 and exp N exc 3. On the basis of the above statistic approach.9nm. is the parameter which proportional to multiplicities of n and a is the atom size.8Еg) we have N exc 7. it is possible to explain the non-Poissonian character of excitons multiplicities. It is important to note that the . n 2 188 that is n 2 (n) 2 n .6 0. R=3. theory 1. S n n n Now we consider application of the above results for MEG in different QDs.g.00 exp which is in a good agreement with the experiment ( N exc 2.

overlapping integral is different from zero due to strong electron-electron correlation in quantum dots. the photon energy. Phys. 549 (1978) 13. Rashidova S. ―High efficient multiple excition generation in colloidal PbSe and PbS quantum dots‖.W. References 1. D. 189. Klimov V. Petruska M.87. ―Nanocrystal Quantum Dots: From fundamental photophysics to multicolor lasing‖.2003. DC.. Rev. Department of Energy (DOE). 1982.I. Lett. Second Printing: U. Lett. 3.S. 9..19.. Nucl. № 8.. 214. 2004..D.I. the gap energy. Nano Lett. 2005.by M.. v. 18021.D. Beard M. Oksengendler B.M. 6. 11... Schaller R. 2002 2. To explain the effect at macroscopic level we have proposed developed an approach consisting of the combination of statistics and Fermi approach to multiple particle generation in high energy nucleon-nucleon collisions. 8. Electrochem.. J. Klimov V. Jonson J.. ―Quantum dot solar cells‖. Mikhailovsky A.J. Appl. 865. Fermi E. ―Basic research needs for solar Energy Utiligation‖. Phys. 2005. Turaeva N.. KlimovV.. Lewis N. Phys. 5. J. Our approach is based on the simple assumption that the probability of n particles generation in the volume QDs is defined by the statistic weight S(n). Matveev V. ―Effect of electronic structure on carrier multiplication efficiency: Comparative study of PbSe and CdSe nanocrystals‖..Nauk. № 3. 1995 . 1950. Agranovich V. 12. ―High-efficiency carrier multiplication through direct photogeneration of multi-exciton via virtual single-exciton‖. Leburton. Dykhne A M and Yudin D L Sov. 14.. ―Statistic Theory of Multiple Exciton generation in Quantum Dots‖.D..I. Klimov V.A. v. et al. Schaller R. Klimov V. 573. Cahay.. v. v. v.A.. v.92. 097402.. Shaking at electronic transitions in atoms. Hollingsworth A. Prog. 7. v. electron and hole effective masses. 2005. 10. 2005. Appl.N. 2001.S.. 329.I.—Usp.. In: ―Quantum Confinement: Nanostructured Materials and Devices‖. Schaller R. ―Non-Poissonian Electron population in Semiconductor Nanocrystals via carrier multiplication‖..D.C. ―Stimulated Emission and Lasing in Nanocrystal Quantum Dots‖. 14. 2009. Such a mechanism allows take into account the strong electron-electron correlation in QDs caused by quantum confinement of electronic excitations. 570. Soc. ―High efficient carrier multiplication in PbSe nanocrystals: Implication for solar energy conservation‖. Nozik A. 5.96. Ed. Phys. the exciton bind energy.1. Crabtree G.138. Lockwood. v. Nature Phys.. Proc. v. Schaller R.Phys. Office of Basic Energy Science. Matveev V I Phys. 2006. Washington.S. The microscopic mechanism of MEG which is based on the electrons shaking theory in atomic collisions is developed. Ellingson R. Lett. Klimov V. Part. Los Alamos Science... 21. Conclusion Thus we have treated multiple electron generation in quantum dots induced by one-photon absorption. Usp.L. Rev. 5. Phyica E.. et al. Phys.I. Solar Energy. 115. 186601. 4. Parilis E.S. 26. 253102. ―Nuclear Processes at High Energy‖. 36. 321.I.I. which depends on many parameters: the size of QD. Theor. In: ―Report of the Basic Energy Science Workshop on Solar Energy Utilization‖. v.

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