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In contrast to the original Kohn-Sham (KS) formalism, we propose a density functional theory (DFT) with fractional orbital occupations for the study of ground states of many-electron systems, wherein strong static correlation is shown to be…

Chemical Physics · Physics 2015-06-03 Jeng-Da Chai

We show that the analytic structure of the dynamical xc kernels of semiconductors and insulators can be sensed in terms of its poles which mark physically relevant frequencies of the system where the counter-phase motion of discrete…

Materials Science · Physics 2023-04-19 D. R. Gulevich , Ya. V. Zhumagulov , V. Kozin , I. V. Tokatly

We calculate the optical spectra of silicon and germanium in the adiabatic time-dependent density functional formalism, making use of kinetic energy density-dependent (meta-GGA) exchange-correlation functionals. We find excellent agreement…

Strongly Correlated Electrons · Physics 2011-11-16 V. U. Nazarov , G. Vignale

A simple, novel, non-empirical, constraint-based orbital-free generalized gradient approximation (GGA) non-interacting kinetic energy density functional is presented along with illustrative applications. The innovation is adaptation of…

Chemical Physics · Physics 2018-08-01 K. Luo , V. V. Karasiev , S. B. Trickey

The primary computational challenge when simulating nonadiabatic ab initio molecular dynamics is the unfavorable compute costs of electronic structure calculations with molecular size. Simple electronic structure theories, like…

Chemical Physics · Physics 2023-06-28 Justin J. Talbot , Martin Head-Gordon , Stephen J. Cotton

Charge transfer plays a crucial role in many processes of interest in physics, chemistry, and bio-chemistry. In many applications the size of the systems involved calls for time-dependent density functional theory (TDDFT) to be used in…

Chemical Physics · Physics 2017-10-11 Neepa T. Maitra

Time-dependent density-functional theory (TDDFT) is deemed to be a formally rigorous way of dealing with the time-evolution of a many-electron system at the level of electron densities rather than the underlying wavefunctions, which in turn…

Chemical Physics · Physics 2024-11-26 Jochen Schirmer

The Tamm-Dancoff Approximation (TDA) offers a computationally efficient alternative to full linear-response Time-Dependent Density Functional Theory (TDDFT) for calculating electronic excited states, particularly in large molecular systems.…

Chemical Physics · Physics 2025-07-02 Muhammed A. Dada , Sarah Pak , Matthew N. Ward , Megan Simons , Daniel R. Nascimento

This chapter provides a basic introduction to excited-state extensions of density functional theory (DFT), including time-dependent (TD-)DFT in both its linear-response and its explicitly time-dependent formulations. As applied to the…

Chemical Physics · Physics 2023-05-02 John M. Herbert

Time-dependent density functional theory (TDDFT) is a theory that describes the time evolution of quantum mechanical many-electron systems under the influence of external time-dependent electric and magnetic fields. INQ is a specially…

We propose a machine learning based approach to develop the exchange-correlation potential of time dependent density functional theory (TDDFT). The neural network projection from the time-varying electron densities to the corresponding…

Computational Physics · Physics 2020-05-20 Yasumitsu Suzuki , Ryo Nagai , Jun Haruyama

For orbital-free {\it ab initio} molecular dynamics, especially on systems in extreme thermodynamic conditions, we provide the first pseudo-potential-adapted generalized gradient approximation (GGA) functional for the non-interacting free…

Chemical Physics · Physics 2020-02-19 Kai Luo , Valentin V. Karasiev , S. B. Trickey

Many-body electron-hole interactions are essential for understanding non-linear optical processes and ultrafast spectroscopy of materials. Recent first principles approaches based on nonequilibrium Green's function formalisms, such as the…

Computational Physics · Physics 2025-02-11 Bowen Hou , Jinyuan Wu , Victor Chang Lee , Jiaxuan Guo , Luna Y. Liu , Diana Y. Qiu

Time-Dependent Density Functional Theory (TDDFT) has been currently established as a computationally cheaper, yet effective, alternative to the Many-Body Perturbation Theory (MBPT) for calculating the optical properties of solids. Within…

Materials Science · Physics 2026-04-13 M. Arruabarrena , A. Leonardo , A. Ayuela

The exchange-correlation (XC) functional in density functional theory is used to approximate multi-electron interactions. A plethora of different functionals is available, but nearly all are based on the hierarchy of inputs commonly…

Time-Dependent Density Functional Theory (TDDFT) has recently been extended to describe many-body open quantum systems (OQS) evolving under non-unitary dynamics according to a quantum master equation. In the master equation approach,…

Chemical Physics · Physics 2015-05-18 David G. Tempel , Mark A. Watson , Roberto Olivares-Amaya , Alán Aspuru-Guzik

While the variational principle for excited-state energies leads to a route to obtaining excited-state densities from time-dependent density functional theory, relatively little attention has been paid to the quality of the resulting…

Chemical Physics · Physics 2025-09-12 Anna Baranova , Neepa T. Maitra

An approximate solution to the time-dependent density functional theory (TDDFT) response equations for finite systems is developed, yielding corrections to the single-pole approximation. These explain why allowed Kohn-Sham transition…

Materials Science · Physics 2009-11-07 H. Appel , E. K. U. Gross , K. Burke

F.E. Harris has been a significant partner in our work on orbital-free density functional approximations for use in ab initio molecular dynamics. Here we mention briefly the essential progress on single-point functionals since our original…

Chemical Physics · Physics 2016-01-12 Valentin V. Karasiev , S. B. Trickey

Energy functionals serve as the basis for different models and methods in quantum and classical many-particle physics. Arguably, one of the most successful and widely used approaches in material science at both ambient and extreme…

Plasma Physics · Physics 2024-10-22 Z. Moldabekov , J. Vorberger , T. Dornheim