Ensemble Time-Dependent Density Functional Theory

Fuente: arXiv
Saved in:
Bibliographic Details
Main Authors: Daas, Kimberly J., Crisostomo, Steven, Burke, Kieron
Format: Preprint
Published: 2025
Subjects:
Online Access:
Tags: Add Tag
No Tags, Be the first to tag this record!
_version_ 1866913151442747392
author Daas, Kimberly J.
Crisostomo, Steven
Burke, Kieron
author_facet Daas, Kimberly J.
Crisostomo, Steven
Burke, Kieron
contents Time-dependent density functional theory (TDDFT) is a standard approach for calculating optical excitations of molecules and solids, while ensemble DFT (EDFT) is a promising alternative under development. We introduce ensemble TDDFT (ETDDFT), a practical theory that combines the two, generalizing both; we ensemble-generalize the Gross-Kohn equation and the exchange-correlation kernel of TDDFT, and generalize EDFT to time-dependent problems. We relate coordinate scaling to the adiabatic connection. The new theory provides multiple avenues for constructing and using approximations. We illustrate these on the 2-site Hubbard model. We connect our results to the more general case of non-perturbative time-dependence.
format Preprint
id arxiv_https___arxiv_org_abs_2507_19464
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Ensemble Time-Dependent Density Functional Theory
Daas, Kimberly J.
Crisostomo, Steven
Burke, Kieron
Chemical Physics
Time-dependent density functional theory (TDDFT) is a standard approach for calculating optical excitations of molecules and solids, while ensemble DFT (EDFT) is a promising alternative under development. We introduce ensemble TDDFT (ETDDFT), a practical theory that combines the two, generalizing both; we ensemble-generalize the Gross-Kohn equation and the exchange-correlation kernel of TDDFT, and generalize EDFT to time-dependent problems. We relate coordinate scaling to the adiabatic connection. The new theory provides multiple avenues for constructing and using approximations. We illustrate these on the 2-site Hubbard model. We connect our results to the more general case of non-perturbative time-dependence.
title Ensemble Time-Dependent Density Functional Theory
topic Chemical Physics
url https://arxiv.org/abs/2507.19464