band gap using molecular dynamics

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I.V. Kityk

a

a, )

Solid State Department of Czestochowa, Uniersityt WSP, Ul. Gombrowicza 1 r 144, PL-42217 Cze stochowa, Poland b Military Technical Academy of Warsaw, ul. Kaliska 4, Warsaw, Poland c Laboratoire de Physique de lEtat Condense UPRES-A6087, Uniersite du Maine, Aenue Oliier Messiaen, F-72085 Le Mans Cedex 9, France Received 29 October 1999; received in revised form 23 November 1999; accepted 14 December 1999 Communicated by L.J. Sham

Abstract The and energy structure of large-sized SiC nanocomposites above 10 nm. was calculated. We used self-consistent norm-conserving pseudopotential method and molecular dynamics simulations of the nanocrystallite interface geometry. Essential changes of the band energy parameters versus the nanocrystallite sizes have been observed. Molecular dynamics structural simulations allowed to find a relation between the degree of hexagonality H relative presence of hexagonal-like phase. and the sizes. Evaluated size-dependent behavior of the energy gap is compared with the experimentally obtained results. Theoretical data have been compared also with experimental optical spectroscopy and X-ray diffraction measurements. The experimental data are in a good agreement with theoretically calculated data. q 2000 Elsevier Science B.V. All rights reserved.

Keywords: Band energy structure; Norm-conserving pseudopotential nanocrystallites; SiC

1. Introduction Recently, one can observe increasing interest to semiconducting nanocrystals due to the striking size-dependent electronic and optical properties w1 6x. There are many investigations devoted to changes of the band structure due to confinement-induced quantization of the continuous band states w7,8x. Traditionally a main experimental method for study of the nanocrystallites consists in using of different optical methods: fluorescence w9x, Raman scattering w10x, photon echo w11,12x, electroluminescence and absorption w13,14x etc. All these works demonstrate

)

an influence of the crystalline size decrease on the changes of the electronic structure and the corresponding optical spectra w15,16x. This is due to the size scaling of electronic transitions and electron phonon interactions w24x, including anharmonic electronphonon interactions w8x. All the known theoretical methods can be classified into two main groups. The first one, consider the crystalline from the long-range ordering solid state approach w17x. Most of the calculations within a framework of the bulk-like approach are done using the semi-empirical band energy calculations. In the second category, the nanocrystals are built as a large molecule and molecular cluster approach is applied w18x. Both of the approaches have the main drawback connected with correct taking into account of coexis-

0375-9601r00r$ - see front matter q 2000 Elsevier Science B.V. All rights reserved. PII: S 0 3 7 5 - 9 6 0 1 9 9 . 0 0 9 1 2 - 3

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tence between the long-range order and local disordering, particularly near the interfaces. Quasiparticle gaps, self-energy corrections, exciton Coulomb energies, and optical gaps in quantum dots were calculated w19x also from first principles using a real space pseudopotential method. The evaluations were performed on spherical clusters possessing up to 800 Si and H atoms. It was demonstrated that the self-energy correction in quantum dots is enhanced substantially compared to bulk, and is not size independent as implicitly assumed in all semiempirical calculations, and quantum confinement and reduced electronic screening results in appreciable excitonic Coulomb energies. A good agreement between the optical gaps calculated within the mentioned framework and experimentally measured prove that the adopted approach really reflects essential influence of the size effect in the large bulk-like clusters. A particular importance is the influence of the nanocrystallite sizes on the nonlinear optical properties w11,12x. A special interest is present in the so-called large-sized nanocrystals larger than 10 nm. w7x. They are from one side nanocrystals and possess size-confinement effects and from the others they have the properties typical for the bulks that allows an introducing the k-dispersion. Such materials are interesting for searching of materials with the enhanced nonlinear optical response susceptibilities because we have contributions originating both from the band states as well from discrete resonance-like levels. The main goal of the present work consists in theoretical simulations of the structural and band energy structure parameters of the real SiC nanocomposites depending on their geometry sizes. In order to test a reliability of the performed calculations comparison with experimental data on the energy gap and the nanocrystallite sizes is presented. In the Section 2 experimental details concerning the SiC nanomaterial specimen preparation are presented. Section 3 is devoted to molecular dynamics geometry optimization of the particular SiC nanoclusters. Norm-conserving pseudopotential method within the local density functional approximation LDFA. used for the size-dependent band energy calculations is described in the Section 4. Calculated size-dependent band energy structure is presented.

Section 5 presents comparison of the theoretically calculated with the experimentally evaluated energy gaps.

2. Experimental The SiC nanopowders were synthesized by a CO 2 laser pyrolysis from a gaseous mixture of SiH 4 and C 2 H 2 following the technology procedure described elsewhere w20x. Annealing of these powders has been performed during 1 h using a high temperature graphite furnace in Ar atmosphere. In the result of such heat treatment, different structural modifications, a coalescence of the SiC grains and a removal of free carbon have been obtained w21x. The critical annealing temperature Ta s 1500 ( C induces some drastic changes of the SiC structure, grain morphology and network composition. It is worth outlining the manifestation of a substantial electric conductivity s f 20Sm -1 at Ta . Varying the mentioned parameters the SiC nanocrystallites of different sizes have been obtained. The specimens had powder-like shape consisting from the proper nanocrystals 435 nm. embedded within the grains of the sizes lying within the 2575 nm. The later are surrounded by amorphous-like SiC background see Fig. 1.. Investigations of a short-range order have been performed by 29 Si and 13 C MAS NMR with large pulse periods in order to sample correctly the material. The NMR characterizations of the materials clearly show a coexistence of b-SiC and a-SiC 6 H or 15 R . structures with a different ratio of SiC admixture in a minor concentration F 10%. SiC.

Fig. 1. Principal geometry structure of the SiC nanocomposites built from the TEM data.

405

Many physical properties of the material are modified due to enhancement of the different kind of vacancies w22x. The energy gap has been measured using the optical absorption and photoconductivity near the absorption edge w23x. Structural parameters have been analyzed using the X-ray diffractometer DRON-3M.

3. Molecular dynamics structure optimization To perform the geometry optimization we applied the molecular dynamics technique described in the Ref. w2426x. We also used several approaches from the molecular dynamics Becke methods w27x involving a semi-empirical contribution of the exact exchange. The mentioned method possess relatively higher convergence with respect to the sizes of the basis sets and allows to vary continuously the intraas well as the inter-cluster distances playing a central role in corresponding structures. In the case of the SiC amorphous-like disordered systems we have used the Green function variation procedure developed well for the glasses w28x.

Fig. 3. Calculated dependence of the degree of hexagonality H versus the nanocrystalline d . and grain L. sizes.

The geometry optimization is started from the interface between the nanocrystallite and amorphous-like background indicated by the dotted line in the Fig. 2.. We began with the molecular dynamics interface simulation of the fourths neighboring layers two from the crystallite sides and two from the amorphous-like sides.. The corresponding levels are indicated by 2, 1, 1 and 2 see Fig. 2.. So we have taken into account about 3040 atoms from the both sides. The molecular dynamics procedure has been performed up to achievement of the total minimum per molecule. in the chosen cluster the same as in the whole composites. The later was determined as a partial sum of the crystallite with the given arb SiC ratio and amorphous-like background. In the second step we consider the layers 3, 2, and 1 and repeat the procedure for the new total partial energy per molecule that corresponds to the new volume of effective supercell due to the restriction of the effective nanocrystallite.. The step-by-step procedure was repeated as an iteration until the relative displacements of the successive layers was That corresponds to atom position less than 0.4 A. precision of the adopted model. We have found that for achievement of the molecular dynamics geometry convergence it is necessary to take into account from 4 up to 7 such layers depending on the degree of hexagonality H and geometry sizes d and L.. The main condition that should be ensured on each step of the molecular basis renormalization is

406

Table 1 Structural parameters of the investigated SiC data: d s sizes of the particular nanoparticles in nm.; L s sizes of the grains in nm.; H s degree of hexagonality. The parameters of the averaged dispersion of the sizes are given in brackets. Specimen 1 2 3 4 5 6 d nm. 13.20.2. 14.40.2. 16.80.2. 19.10.2. 220.2. 260.2. L nm. 320.2. 570.2. 660.2. 560.2. 380.2. 320.2. H 0.04 0.220.2. 0.350.2. 0.610.2. 0.770.2. 0.920.2.

energy is expressed within the framework of the LDFA approximation and is performed with respect to charge density r (r) w29x. The pseudopotential was chosen in the form introduced in the Ref. w29x:

b ,l . 2 b Vps r . s S i A ib , q r A iq 3

=exp ya 1 l , b . r .

1.

the condition of the constant total energy per molecule. That is similar to the well-known dynamics boundary derivative procedure of Broyden FletcherGoldfarbShanoo w2426x with variable effective cluster sizes dynamics boundary conditions. and requirement of the total energy minimum saving. From the total energy the more probable cluster configurations have been found. In Fig. 3 methods dependencies of the degree of hexagonality H partial presence of the hexagonal-like phase determined by the X-ray diffraction method. are shown evaluated by the described above versus the nanocrystalline d and grain L sizes. The general behavior shows a good agreement between the experimental and theoretical data compare Table 1 and Fig. 3.. Several discrepancies in the values reflect probably a coexistence of the different structural fragments for the real composites. One can see an appearance of a maximum of the H for the grain sizes about 34 nm. It is caused by an appearance of the so-called sizeresonance confinement effect between the nanoparticles and grains. Simultaneously, one can see an existence of another maximum for the nanoparticle sizes about 25 nm. The performed calculations indicate that origin of the maxima is caused mainly by a competition between the intracrystalline long-range order and surrounding amorphous-like background.

4. Methods of norm-conserving pseudopotential band energy structure calculations Starting pseudowavefunctions for the non-local norm-conserving pseudopotential were built using the procedure proposed in the Ref. w26x. The total

Such a form allows obtaining the corresponding matrix elements analytically. The detailed expressions for the corresponding matrix elements are presented in the Ref. w30x. All the consideration is carried out for the hexagonal Brillouine zone. The superposition of the different structural fragments has been successfully used for the binary solid alloys w31x, glasses and organic materials w32x. Generally, this approach may be sufficient for the different disordered materials and partially ordered solids. The investigated SiC nanocrystallites may be considered as a partial case of this kind of systems. We have chosen the plane wave basis set with a cutoff up to 335 Ry to achieve the eigenvalues convergence up to 0.02 eV in accordance with the calculations performed in the Ref. w32x. Solving the secular equation is carried out using the Querry limited method with the adding of the 3050 additional plane waves in the Lowdin perturbation approach to carry out the calculations in a more extended plane wave basis set. Electron screening effects were calculated using the CeperleyAlder expression w33x parameterised by PerdewZunger w34x. The special k-point method of ChadhiCohen w35x was used to calculate the space electron charge density distribution. The latter is used to construct a charge density functional for electrons. The diagonalisation procedure was performed at special points of the each structural type. Acceleration of the iteration convergence was achieved by mixing the m-1.th iteration with 70% of the output r before their substitution into the next equation. A criterion of the self-consistency consists in the fulfilling of condition: < rout ,m y r in ,m < - 2. after the mth iteration step. We assumed an accuracy better than s 0.10% between the input and output iterations as a main criterion of the self-consistency.

407

In order to study how the results of the energy band calculations depend on the choice of the aSiCrb-SiC ratio we have carried out test calculations for the pure and a-SiC and b-SiC crystalline phases. An agreement with the calculations of the density of states within the LMTO or pseudoptential methods w36x was up to 0.1 eV. However, the main drawback of all the one-electron calculations consists in the underestimation of the band gaps. Therefore during the energy gap calculations the self-energy effects on the one-electron approach have been superimposed. The electron structure of the amorphous background has been calculated using the quantum chemical simulations for the randomly oriented background described by us in the Ref. w37x. Cluster size termination determining boundary conditions. in this case has been done using X-ray diffractometry data. In the real nano-powder structure we used the approach developed for the solids with the simultaneous presence of the different degree of ordering w32,38x. As a consequence, the effective potential was presented as a superposition of the amorphouslike long-range background inter-grain regions and local nanocrystallite contributions: V G . s 1rV am

lites; V am r . and V cryst r . are the potentials corresponding to the amorphous-like and crystallites states, respectively.

5. Size-dependent band energy structure The performed self-consistent band energy structure calculations have shown that the minimum of the total energy Utot per molecule depends on the degree of hexagonality H. From the Table 2 one can see that the Utot possess a minimum of about 40.13 eV. at degree of hexagonality H about 0.56. All the evaluations were performed for the typical nanocrystallite geometry equal to d s 20 nm and L s 30 nm. An example of the contributions of the nanocrystallite with different sizes to the band energy structure features is presented in Fig. 4. From the presented band energy structure there exist a possibility to determine the contributions of the different effective basic nanocrystals into the central hexagonal quasi-Brillouine zone. All the notation of the symmetry points are generally adopted. Comparing with the bulk crystals we should point out more flat features of the particular bands. The second consequence consists in a variation of the effective energy gap with a change of the effective nano-cluster sizes. However, effective mass, which is connected with the energy dispersions is not changed essentially. All the calculations were performed within the 356 points of the BZ. During the self-consistent band LDFA calculation procedure all the occupied states starting from 1s one were included. In addition, we took into account the excited CI states up to the 32 eV higher than the vacuum energy level.

Hg

am

V am r . exp yi G P r . d 3 r

cr

q 1rV cr

Hg

V cr r . exp yi G P r . d 3 r ,

3.

where G corresponds to the plane-wavevector within the wurtzite-like hexagonal BZ; g am and g cr correspond to the weighting factors directly connected with the concentrations of the proper nanocrystal-

Table 2 Variations of the minimum of the total energy per molecule Utot versus degree of hexagonality for the bulk crystals, amorphous-like background and of the nanocrystallittes after the geometry optimisation. Degree of hexagonality, H 0.24 0.36 0.56 0.75 0.89 Total energy of the SiC per molecule Utot of the bulk Utot of the amorphous crystals weVx SiC background weVx y38.24 y39.56 y40.13 y39.94 y39.87 y35.13 y35.13 y35.13 y35.13 y35.13 Utot of the nanocrystallittes after the geometry optimisation weVx y47.13 y48.56 y48.74 y48.05 y47.96

408

Fig. 4. Effective band energy structure of the SiC nanocrystals showing contributions of clusters with different degree of hexagonality H to the wurtzite-like hexagonal Brillouine zone: ___ 0.84; rrr 0.42; v 0.73; B 0.25.

From Fig. 4 one can see an essential difference in the E(k) dispersion behavior for the sub-bands in the SiC crystallites of different sizes. The band energy k-wavevector dispersion is similar for the G K and KM directions of the BZ. A slight break in the wurtzite-like symmetry probably reflects an appearance of the environment amorphous-like disturbance. Decrease of the particle sizes leads to the flatter and narrower bands. k-dispersion of the upper valence band for the G H direction is essentially less. The latter one reflects an increase of the hole carrier localization due to a decrease of the cluster sizes. Different background corresponds to band energy k-dispersion originating from the different nanocluster sizes. From the presented data one can clearly see that within the presented approach we can to determine the particular contributions of the different effective subclusters into the band energy structure. Simultaneously we are able to evaluate the effective masses originating from the different subbands. Such approach could be very useful for all the particular cases of the partially disordered crystallites. The interfaces play substantial role in such kinds of the composites. As a consequence the competition between the ordered highly-organized. and disordered system is observed.

sizes it is difficult to estimate a type of the inter-band transitions. From the performed calculations we have obtained energy gaps dependence of the interface layer for the averaged nanoparticle sizes see Fig. 5.. Dependence of the energy gaps versus the nanocrystallite d . and grain L. sizes is essentially non-linear. This fact could be used for prediction of the optical and electronic properties of the SiC nanocrystallites. This one indicates also a difference between the ordered intra-particle oriented potential and less negative disordered environment potential. From Fig. 5 one can see nonlinear dependence of the effective energy gap versus nanocrystalline-grain dL. sizes. With decreasing grain sizes below the 65 nm there appears a maximum in the energy gap at d s 14 nm and minimum at d s 19.6 nm. A difference between the maxima and the minima increases from 0.21 eV at L s 60 nm up to 0.93 eV at d s 30 nm. The observed dependence is the result of competition between the intracrystalline range order and surrounding amorphous-like disorder because neglecting by such substructure does not show the calculated modulated-like dependence of the energy gap. Moreover, such a behavior may be general for all the nanocrystallite-like materials forming the grains. The performed investigations show that the sizes of the nanocrystallites d and L. are unambiguously connected with degree of hexagonality H. Therefore to avoid complicated presentation versus the d, L parameters the appropriate arguments d, L. have been replaced by a degree of hexagonality H. As a

6. Energy gaps behavior The calculated energy band gaps were of the direct type but for the decreasing nano-crystalline

Fig. 5. Dependence of effective energy gap Eg on nanoparticle d and grain L sizes obtained from the theoretical simulations.

409

At the same time direct relation between the SiC geometry and degree of the hexagonality H has been revealed. Anomalies of the electronic and structural properties near the resonance of the nanocrystals and grain sizes reflect a competition between the longrange-ordering in the nanocrystallites and surrounding grains. A good agreement of the size-dependent energy gap calculated theoretically and measured experimentally indicates on a possibility of applying such approach for the large-sized nanocrystallites.

Acknowledgements The authors are akcnowledged to Professor M. Cauhetier CEA, France. for the support of the work.

Fig. 6. Experimental dependence of the energy gap versus the degree of hexagonality H.

References consequence in the Fig. 6 are presented dependencies of the effective energy gap versus degree of hexagonality H. Comparing the Table 1 connecting the hexagonality H with the evaluated size dimensions d, L. one can see satisfactory agreement in the general tendency. However, several discrepancies up to 15%. exist in the absolute values of energy gaps. These once can be caused by a non-an inaccuracy of the experimental measurements of the energy gap in the SiC nanocomposites.

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7. Conclusions The band energy for the SiC nanocrystallites with large sizes was calculated using the norm-conserving pseudopotential calculations within a framework of the LFDA approach. and molecular dynamics interface geometry optimizations as a function of the nanocrystallite sizes d, L.. Decreasing hexagonality H induces an increase of the energy gap. The energy gap is strictly connected with sizes of the grains L and of the particular nanoparticles L. Decreasing of the grain size L. causes increasing energy gap. The smallest values of the SiC energy gaps have been observed for the nanoparticle sizes of about 2025 nm.

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I.V. Kityk et al. r Physics Letters A 265 (2000) 403410 w30x I.V. Kityk, J. Kasperczyk, B.V. Andrievskii, Phys. Lett. A 216 1996. 161. w31x M. Malachowski, I.R. Kityk, B. Sahraoui, Phys. Lett. A 242 1998. 337. w32x B. Sahraoui, I.V. Kityk, X. Nguyen Phu, P. Hudhomme, A. Gorgues, Phys. Rev. B 59 1999. 9229. w33x P. Zhang, Doctoral dissertation, Shanghai Jiao Tong University, China, 1998, unpublished. w34x J.B. Perdew, A. Zunger, Phys. Rev. B 23 1981. 5048. w35x D.J. Chadi, M.L. Cohen, Phys. Rev. B 8 1973. 5747. w36x P. Zhang, Doctoral dissertation, Shanghai Jiao Tong University, China, 1998, unpublished. w37x E. Fu, E. Yaschenko, L. Resca, K. Resta, Solid State Commun. 112 1999. 465. w38x I.V. Kityk, E. Jakubczyk, Z. Mandecki, Mater. Sci. & Eng. A 134 1997. 1045.

w19x S. Ogut, J.R. Chelikowsky, Phys. Rev. Lett. 79 1997. 1770. w20x M. Cauchetier, O. Cloix, M. Luce, Adv. Ceram. Mater. 36 1988. 548. w21x S. Charpentier Ph.D. thesisUniversite du Maine 1998.. w22x S. Charpentier, A. Kassiba, J. Emery, M. Cauhetier, J. Phys.: Cond. Matter 11 1999. 4887. w23x J. Pankove, Optical Properties of Semiconductors, NY, Academic, 1969. w24x P. Zhang, Doctoral dissertation, Shanghai Jiao Tong University, China, 1998, unpublished. w25x D. Goldfarb, Math. Comput. 24 1970. 23. w26x D.F. Shanoo, Math. Comput. 24 1970. 647. w27x A.D. Becke, J. Chem. Phys. 1372 98 1994. 5648. w28x P. Hohenberg, W. Kohn, Phys. Rev. 136 1964. 864. w29x P. Zhang, Doctoral dissertation, Shanghai Jiao Tong University, China, 1998, unpublished.

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