Abstract
The electronic properties of silicon nanostructures are calculated using a timedependent algorithm within the tight-binding approximation. The algorithm includes the electron-hole Coulomb interaction directly without resort to perturbative correction, allowing accurate calculation of excited state properties. The densities of states, fundamental band gaps, photoluminescence energies, and band edge eigenfunctions andk-distributions are calculated for nanostructures up to 100Å in diameter. The effects of size, geometry, surface termination, and surface reconstruction on the electronic properties are investigated. We show that a model in which the primary photoluminescence peak is due to exciton recombination across the fundamental gap, while the secondary infra-red peak is due to recombination of a conduction band electron with a hole in a deep surface trap is consistent with recent observations for both silicon nanocrystals and porous silicon. We infer the geometry of the luminescent region in porous silicon by comparing our calculated results with experimental data on porous silicon samples.
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References
L.T. Canham,Appl. Phys. Lett. 57, 1046 (1990).
S. Schuppler, S.L. Friedman, M.A. Marcus, D.L. Aider, Y.-H. Xie, F.M. Ross, T.D. Harris, W.L. Brown, Y.J. Chabal, L.E. Brus and P.H. Citrin,Phys. Rev. Lett. 72, 2648 (1994).
D.J. Calcott, K.J. Nash, L.T. Canham, M.J. Kane and D. Brumhead,J. Lum. 57, 257 (1993).
F. Koch, V. Petrova-Koch and T. Muschik,J. hum. 57, 271 (1993).
Other models based on molecular recombination in species such as polysilanes (S.M. Prokes, O.J. Glembocki, V.M. Bermudez, R. Kaplan, L.E. Friedersdorft and P.C. Searson,Phys. Rev. B 45,13788 [1992]) or siloxenes (M.S. Brandt, H.D. Fuchs, M. Stutzman, J. Weber and M. Cardona,Solid State Commun. 81, 307 [1992]) are not widely accepted.
E. Martin, C. Delerue, G. Allan and M. Lannoo,Phys. Rev. 50, 18258 (1994).
N.A. Hill and KB. Whaley,J. Chem. Phys. 99, 3707 (1993).
N.A. Hill and KB. Whaley,J. Chem. Phys. 100,2831 (1994).
N.A. Hill and KB. Whaley, submitted.
P. Vogl, H.P. Hjalmarson and J.D. Dow,J. Phys. Chem. Solids 44, 365(1983).
J.R. Chelikowsky and M.L. Cohen,Phys. Rev. 14,556 (1976).
H. Basch, A. Viste and H.B. Gray,Theoret. Chim. Acta 3,458 (1965).
M. Wolfsberg and L. Helmholtz,J. Chem. Phys. 20, 837 (1952).
Gaussian Inc., 4415 Fifth Avenue, Pittsburgh, PA 15213.
J.C. Slater,Phys. Rev. B 36, 57 (1930).
K. Schulten, I. Ohmine and M. Karplus,J. Chem. Phys. 64, 4422 (1976).
K. Ohno,Theoret. Chim. Acta 2, 219 (1964).
Z.H. Levine and S.G. Louie,Phys. Rev. B 25, 6310 (1982).
L.W. Wang and A. Zunger,Phys. Rev. Lett. 73, 1039 (1994).
L.E. Brus,J. Chem. Phys. 80, 4403 (1984).
N.A. Hill and KB. Whaley,Phys. Rev. Lett. 75, 1130 (1995).
S. Schuppler et al.,Phys. Rev. B 52, 4910 (1995).
V. Petrova-Koch, private communication.
L.E. Brus, P.F. Szajowski, W.L. Wilson, T.D. Harris, S. Schuppler and P.H. Citrin,J. Am. Chem. Soc. 117, 2915 (1995).
T. Suemoto, K Tanaka and A. Nakajima,J. Phys. Soc. Jpn. 63 B, 190 (1994).
M.V. Rama Krishna and R.A. Friesner,J. Chem. Phys. 96, 873 (1992).
L.W. Wang and A. Zunger,J. Phys. Chem. 98, 2158 (1994).
T. Uda and M. Hirao,J. Phys. Soc. Jpn. 63 Suppl. B, 97 (1994).
S.Y. Ren and J.D. Dow,Phys. Rev. B 45, 6492 (1992).
C. Delerue, G. Allan and M. Lannoo,Phys. Rev. B 48, 11024 (1993).
T. Kakagahara and K. Takeda,Phys. Rev. B46,15578(1992).
M.S. Hybertsen,Phys. Rev. Lett. 72, 1514 (1994).
Z. Jing and J.L. Whitten,Phys. Rev. B 46, 9544 (1992).
E. Kaxiras and J.D. Joannopoulos,Phys. Rev. B 37, 8842 (1988).
J.C. Slater and G.F. Koster,Phys. Rev. 94, 1498 (1954).
The same effect was observed for CdSe nanocrystals. 8
J.R. Heath and P.E. Batson, private communication.
V. Lehman and U. Gösele,Appl. Phys. Lett. 58, 856 (1991).
W. Lang, P. Steiner and F. Kozlowski,J. Lum. 57,341 (1993).
A mixture of wires and crystallites has been postulated in order to bring PP lifetime calculations into agreement with experiment (C.-Y. Yeh, S.B. Zhang, and A. Zunger,Appl. Phys. Lett. 63, 3455 [1993]).
V. Petrova-Koch, T. Muschik, G. Polisski and D. Kovalev,MRS Symposium Proc. 358 (Pittsburgh, PA: MRS, 1995), p. 483.
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Hill, N.A., Whaley, K.B. A theoretical study of light emission from nanoscale silicon. J. Electron. Mater. 25, 269–285 (1996). https://doi.org/10.1007/BF02666256
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DOI: https://doi.org/10.1007/BF02666256