Luis Enrique Rosas-Hernandez

arXiv2025

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

The second-order optical susceptibility of semiconductors $χ_{ijk}^{(2)}(-2ω;ω,ω)$ finds application in metrology, spectroscopy, telecommunications, material characterization, and quantum information. Pioneering calculations of $χ_{ijk}^{(2)}(-2ω;ω,ω)$ 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 ({\em i.e.}, {\em localized}) orbitals, making a comeback onto frameworks based on localized basis sets. Here, we present an approach for calculating $χ_{ijk}^{(2)}(-2ω;ω,ω)$ reliant on numerical pseudoatomic 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.

cond-mat.mtrl-sci↗

arXiv2024

Insulating moiré homobilayers lack a threefold symmetric second harmonic generation

Atoms within moiré bilayers relax in-plane to minimize elastic energy [e.g., Cazeaux et al., J. Elast. 154, 443 (2023)]; such relaxation brings their space group symmetries down to P1. Here, the ab initio second harmonic generation (SHG) of twisted and atomistically optimized hBN bilayers was determined at four twist angles ($θ=38.21^{\circ}$, $60.00^{\circ}$, $73.17^{\circ}$, and $98.21^{\circ}$) and for three displacements $\boldsymbolτ$ measured away from the ground state $AA^{\prime}$ configuration. All moiré bilayers have a P1 space symmetry after structural optimization. This situation is quite different to monolayers with hexagonal lattices, which retain a three-fold symmetry. We point out that the actual symmetries of the SHG reported for hBN bilayers on two experimental works do not coincide with the sixfold symmetric theoretical profiles they provide [either $\sin^2(3ϕ)$ or $\cos^2(3ϕ)$], and show that the intrinsic low structural symmetry of (atomically optimized) hBN bilayer moirés can in fact be read out from experimental SHG intensity profiles--which are tunable by $θ$ and by the frequency of light $ω$: The SHG is most definitely not sixfold-symmetric because moirés do not retain a three-fold symmetry. Furthermore, an extrinsic twofold symmetry of the SHG emission is realized by tilting the pump by an angle $α$ away from the 2D material's normal, regardless of $θ$ and $ω$. The design of in-plane and ultrathin sources of SHG with low symmetry could be useful for the eventual creation of entanglement sources from 2D materials.

cond-mat.mtrl-sci↗