Parameterized Attenuated Exchange for Generalized TDHF@$v_W$ Applications
Abstract
Building upon our previously developed time-dependent Hartree-Fock (TDHF)@ method, based on many-body perturbation theory and specifically the Bethe-Salpeter Equation (BSE), we introduce a parameterization scheme for the attenuated exchange kernel, . In the original method, was determined individually for each system via an efficient stochastic short-time TD Hartree propagation for the screened Coulomb interaction, . The new parameterization leverages photochemical similarities in exciton binding energies (or exchange interaction attenuation) among molecules with comparable static dielectric responses. We parameterize the inverse dielectric function using a low-order polynomial with error function apodization, calibrated on a few representative molecules, each with its own . Using only 7 parameters, the parameterized is fully grid-independent and broadly applicable within a family of molecules. This enables TDHF@ that retains BSE-level accuracy, achieving a mean absolute error of eV compared to experimental optical gaps and representing a five- to ten-fold improvement over conventional TD density functional theory or TDHF while reducing the cost to that of standard TDHF.
Keywords
Cite
@article{arxiv.2504.01285,
title = {Parameterized Attenuated Exchange for Generalized TDHF@$v_W$ Applications},
author = {Barry Y. Li and Tim Duong and Tucker Allen and Nadine C. Bradbury and Justin R. Caram and Daniel Neuhauser},
journal= {arXiv preprint arXiv:2504.01285},
year = {2025}
}