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Recent Advances in ab initio time—dependent Hartree-Fock theory and their applications to predict nonlinear optical properties of semiconductor nanoclusters

Published online by Cambridge University Press:  15 February 2011

Shashi P. Karna  and
Prakashan P. Korambath
Shashi P. Karna
Affiliation:
Air Force Research Laboratory Space Vehicles Directorate 3550 Aberdeen Avenue, Bldg. 914 Kirtland AFB, NM 87117-5776
Prakashan P. Korambath
Affiliation:
Air Force Research Laboratory Space Vehicles Directorate 3550 Aberdeen Avenue, Bldg. 914 Kirtland AFB, NM 87117-5776
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Abstract

Recent advancements in ab initio time-dependent Hartree-Fock (TDHF) theory have made it a technique of choice for modeling nanoscale nonlinear optical (NLO) materials from first-principles. We have used this method to study structure-NLO property relationships of GaN, GaP and GaAs clusters. The geometry of the clusters used in the study was optimized by ab initio Hartree Fock (HF) calculations with the use of even tempered Gaussian (ETG) basis set. The clusters used in this study are of the type Gam Xn (M = 1,3,4,7 and n = 1,3,4,7) where X=N, P, and As. The GamXn clusters are in a charge neutral (q = 0) state for m = n and in appropriately charged state for m ∦ n. The magnitude of the calculated (hyper)polarizabilities appears to strongly depend on the composition of the cluster. For the same composition of heteroatoms, the hyperpolarizability depends on the size as well as the geometry of the cluster. The cluster size-dependence of calculated (hyper)polarizabilities is more pronounced for the first-hyperpolarizability. β than for the polarizability, α The calculated β(–ωμ,ωl,ω2) corresponding to various second order effects shows the following trend β(–2ω; ω,ω) > β(–ω; 0, ω) >β(0;0,0).

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 579: Symposium B – The Optical Properties of Materials , 1999 , 169
Copyright
Copyright © Materials Research Society 2000

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References

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