Perturbative second-order optical susceptibility of bulk materials: a symmetry-enforced return to non-orthogonal localized basis sets

Huamán, Angiolo; Enrique Rosas-Hernandez, Luis; Barraza-Lopez, Salvador

doi:10.1088/1361-648X/ae35fa

Perturbative second-order optical susceptibility of bulk materials: a symmetry-enforced return to non-orthogonal localized basis sets

Journal Article · Fri Jan 30 00:00:00 EST 2026 · Journal of Physics. Condensed Matter

DOI:https://doi.org/10.1088/1361-648X/ae35fa· OSTI ID:3017977

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Univ. of Arkansas, Fayetteville, AR (United States)

The second-order optical susceptibility of semiconductors $$\chi^{(2)}_{ijk}(-2\omega;\omega,\omega)$$ finds application in metrology, spectroscopy, telecommunications, material characterization, and quantum information. Pioneering calculations of $$\chi^{(2)}_{ijk}(-2\omega;\omega,\omega)$$ utilized non-orthogonal Gaussian orbitals centered at atoms. That formulation transitioned into plane-wave-based algorithms as time went by. As of late, nevertheless, multiple tools for calculating optical susceptibilities have recast the problem using Wannier (i.e. localized) orbitals, making a comeback onto frameworks based on localized basis sets. Here, in this work, we present an approach for calculating $$\chi^{(2)}_{ijk}(-2\omega;\omega,\omega)$$ reliant on numerical pseudo-atomic orbitals (PAOs) within perturbation theory in the velocity gauge. Its salient feature is a calculation of ‘Slater–Koster-like’ two-center integrals of the momentum operator in between PAOs identified by symmetry. The approach was successfully tested on paradigmatic cubic silicon carbide (3C-SiC) and gallium arsenide, for which linear responses are contributed as well.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Arkansas, Fayetteville, AR (United States)

Sponsoring Organization:: National Science Foundation; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0022120

OSTI ID:: 3017977

Journal Information:: Journal of Physics. Condensed Matter, Journal Name: Journal of Physics. Condensed Matter Journal Issue: 4 Vol. 38; ISSN 0953-8984; ISSN 1361-648X

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

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