Optica Open
Browse
arXiv.svg (5.58 kB)

Length-gauge optical matrix elements in WIEN2k

Download (5.58 kB)
preprint
posted on 2023-01-12, 14:48 authored by Oleg Rubel, Peter Blaha
Hybrid exchange-correlation functionals provide superior electronic structure and optical properties of semiconductors or insulators as compared to semilocal exchange-correlation potentials due to admixing a portion of the non-local exact exchange potential from a Hartree-Fock theory. Since the non-local potential does not commute with the position operator, the momentum matrix elements do not fully capture the oscillator strength, while the length-gauge velocity matrix elements do. So far, length-gauge velocity matrix elements were not accessible in the all-electron full-potential WIEN2k package. We demonstrate the feasibility of computing length-gauge matrix elements in WIEN2k for a hybrid exchange-correlation functional based on a finite difference approach. To illustrate the implementation we determined matrix elements for optical transitions between the conduction and valence bands in GaAs, GaN, (CH$_3$NH$_3$)PbI$_3$ and a monolayer MoS$_2$. The non-locality of the Hartree-Fock exact exchange potential leads to a strong enhancement of the oscillator strength as noticed recently in calculations employing pseudopotentials [Laurien and Rubel: arXiv:2111.14772 (2021)]. We obtained an analytical expression for the enhancement factor in terms of the difference in eigenvalues not captured by the kinetic energy. It is expected that these results can also be extended to other non-local potentials, e.g., a many-body $GW$ approximation.

History

Disclaimer

This arXiv metadata record was not reviewed or approved by, nor does it necessarily express or reflect the policies or opinions of, arXiv.

Usage metrics

    Categories

    Licence

    Exports

    RefWorks
    BibTeX
    Ref. manager
    Endnote
    DataCite
    NLM
    DC