Bond Model and Group Theory of Second Harmonic Generation in GaAs(001)

TL;DR

This paper compares the Bond Model and Group Theory for second harmonic generation in GaAs(001), demonstrating that the simplified bond hyperpolarizability model can accurately reproduce experimental results with minimal parameters.

Contribution

It extends the SBHM to diatomic crystals like GaAs and shows it aligns well with group theory and experimental data, using only one fitting parameter.

Findings

SBHM can be applied to diatomic crystals like GaAs

Good agreement with experimental SHG data using minimal parameters

Third rank tensor matches group theory predictions

Abstract

A comprehensive analysis of second harmonic generation (SHG) in a diatomic zincblende crystal based on the Simplified Bond Hyperpolarizability Model (SBHM), Group Theory (GT) is presented. The third rank tensor between the two approaches are compared and applied to reproduce rotational anisotropy (RA) SHG experimental result.It is well known that such a crystal is noncentrosymmetric, therefore the second harmonic generation source is dominated by bulk dipoles with a SHG polarization $P_{BD}=\chi_{ijk}^{(2)}E(\omega)E(\omega)$. We show that the SBHM previously applied to mono crystal system such as Silicon can also be applied to an atomic cell containing two different atoms e.g. GaAs by introducing an effective hyperpolarizability $\alpha_{2GaAs}=\left(\alpha_{2Ga}-\alpha_{2As}\right)$ . Comparison with GT yields the same third rank tensor for a $T_d$ point group corresponding to bulk tetrahedral structure. Interestingly, SBHM gives good agreement with RASHG experiment of GaAs using only one single fitting parameter when Fresnel analysis is also incorporated in the model.