All-electron Dynamical Bethe-Salpeter Equation for Extended Systems with Atom-centered Orbital Basis
Abstract
Solving Bethe-Salpeter equation (BSE) for the two-particle Green's function is the most widely used approach for taking into account the particle-hole (exciton) interaction in electronic excitation in the context of the many-body theory based on Green's function. In BSE calculations, the static approximation to the screened Coulomb interaction kernel is commonly employed. However, when the excitonic character is significant as typically indicated by a large exciton binding energy, dynamical screening effects become non-negligible, rendering the static approximation questionable. Because of the large computational cost due to the dense Brillouin zone integration necessary for convergence, solving the dynamical BSE for extended systems remains a significant challenge, especially when combined with GW calculation for the calculation of quasi-particle energies. In this work, we formulate the plane-wave based effective dielectric function method [Zhang, et al., Phys. Rev. B 107, 235205 (2023)] for the dynamical BSE calculation using atom-centered orbitals as basis functions. We implement this approach in our recently developed all-electron numerical atom-centered orbital (NAO) implementation of BSE@GW [Zhou, et. al. J. Chem. Theory Comput. 21, 291 (2025)] for extended systems. We validate our all-electron NAO-based implementation of the dynamical BSE method, and we then discuss its realistic application to molecular crystal of naphthalene by performing the dynamical BSE@G0W0 calculation.
Related
- Real-Time Approach to the Dynamical Bethe-Salpeter Equation for Finite Systems
- Quasiparticle quantum simulation of materials with the Bethe-Salpeter equation
- All-electron RT-TDDFT with Exact Exchange based on Numeric Atom-centered Orbitals for Condensed Matter
- Smart Machine Learning for Solving the Full Electron-Nuclear Schrödinger Equation with a Quantum-Chemically Inspired Wavefunction Ansatz
- Nonuniform Screening Reshapes Collective Excitons in Molecular Aggregates from Stochastic Bethe-Salpeter Theory
BibTeX
@misc{zhou2026allelectron,
title = {{All-electron Dynamical Bethe-Salpeter Equation for Extended Systems with Atom-centered Orbital Basis}},
author = {Ruiyi Zhou and Songrui Liu and Jianhang Xu and Yi Yao and Yosuke Kanai},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2606.08350},
eprint = {2606.08350},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2606.08350},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - All-electron Dynamical Bethe-Salpeter Equation for Extended Systems with Atom-centered Orbital Basis
AU - Ruiyi Zhou
AU - Songrui Liu
AU - Jianhang Xu
AU - Yi Yao
AU - Yosuke Kanai
PY - 2026
DA - 2026/09/10
PB - arXiv
DO - 10.48550/arxiv.2606.08350
UR - https://arxiv.org/abs/2606.08350
AB - Solving Bethe-Salpeter equation (BSE) for the two-particle Green's function is the most widely used approach for taking into account the particle-hole (exciton) interaction in electronic excitation in the context of the many-body theory based on Green's function. In BSE calculations, the static approximation to the screened Coulomb interaction kernel is commonly employed. However, when the excitonic character is significant as typically indicated by a large exciton binding energy, dynamical screening effects become non-negligible, rendering the static approximation questionable. Because of the large computational cost due to the dense Brillouin zone integration necessary for convergence, solving the dynamical BSE for extended systems remains a significant challenge, especially when combined with GW calculation for the calculation of quasi-particle energies. In this work, we formulate the plane-wave based effective dielectric function method [Zhang, et al., Phys. Rev. B 107, 235205 (2023)] for the dynamical BSE calculation using atom-centered orbitals as basis functions. We implement this approach in our recently developed all-electron numerical atom-centered orbital (NAO) implementation of BSE@GW [Zhou, et. al. J. Chem. Theory Comput. 21, 291 (2025)] for extended systems. We validate our all-electron NAO-based implementation of the dynamical BSE method, and we then discuss its realistic application to molecular crystal of naphthalene by performing the dynamical BSE@G0W0 calculation.
ER -