Testing exact-factorization-based density functional approximation on a continuous density model

In this work, we test the performance of an exact-factorization-based density functional approximation (DFA) for electron-nuclear correlation beyond the Born-Oppenheimer approximation that was derived in Li et al. [J. Chem. Phys.148, 084110 (2018)]. The present work extends beyond the Hubbard model that was used previously in a two-electron Shin-Metiu model with continuous electronic density in one dimension. Using new iteration techniques, we managed to solve coupled Kohn-Sham equations that embody nonadiabatic corrections with a nuclear Schrödinger equation. Our results show that the DFA can successfully capture the nonadiabatic effect caused by electron-nuclear correlation as manifested in the correct shift of the critical nuclear position where the proton-coupled electron transfer takes place. The nonadiabatic correction to the Kohn-Sham potential also leads to a shift of orbital energies, which can potentially be useful to study band renormalization induced by electron-phonon interactions in bulk materials.

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Publication Details

Journal
The Journal of Chemical Physics
Published
2025-06-16
DOI
https://doi.org/10.1063/5.0260749
Primary Topic
Advanced Chemical Physics Studies
Type
article
Field-Weighted Citation Impact
0.00

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article

Testing exact-factorization-based density functional approximation on a continuous density model

Y. Li, Chen Li, Zixuan Wang
1 links
The Journal of Chemical Physics
Advanced Chemical Physics Studies
article

Testing exact-factorization-based density functional approximation on a continuous density model

Y. Li, Chen Li, Zixuan Wang
article en

Abstract

In this work, we test the performance of an exact-factorization-based density functional approximation (DFA) for electron-nuclear correlation beyond the Born-Oppenheimer approximation that was derived in Li et al. [J. Chem. Phys.148, 084110 (2018)]. The present work extends beyond the Hubbard model that was used previously in a two-electron Shin-Metiu model with continuous electronic density in one dimension. Using new iteration techniques, we managed to solve coupled Kohn-Sham equations that embody nonadiabatic corrections with a nuclear Schrödinger equation. Our results show that the DFA can successfully capture the nonadiabatic effect caused by electron-nuclear correlation as manifested in the correct shift of the critical nuclear position where the proton-coupled electron transfer takes place. The nonadiabatic correction to the Kohn-Sham potential also leads to a shift of orbital energies, which can potentially be useful to study band renormalization induced by electron-phonon interactions in bulk materials.

The Journal of Chemical PhysicsVol. 162(23)
Peking University (CN), Beijing National Laboratory for Molecular Sciences (CN)
National Natural Science Foundation of China, National Key Research and Development Program of China
Openalex Percentile: Top 89%
Advanced Chemical Physics Studies
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