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This work merges two different types of many-electron ensembles, namely the Theophilou-Gross-Oliveira-Kohn ensembles of ground and neutrally-excited states, and the more recent $N$-centered ensembles of neutral and charged ground states. On…

Chemical Physics · Physics 2024-06-10 Filip Cernatic , Pierre-François Loos , Bruno Senjean , Emmanuel Fromager

We develop a generalization of the Kohn-Sham density functional theory (KS-DFT) + Hubbard $U$ (DFT+$U$) method to the excited-state regime. This has the form of Hubbard $U$ corrected linear-response time-dependent DFT, or `TDDFT+$U$'.…

Strongly Correlated Electrons · Physics 2019-04-24 Okan K. Orhan , David D. O'Regan

A combination of classical molecular dynamics (MM/MD) and quantum chemical calculations based on the density functional theory (DFT) was performed to describe conformational properties of diphenylethyne (DPE), methylated-DPE and poly para…

Mesoscale and Nanoscale Physics · Physics 2016-12-21 Behnaz Bagheri , Björn Baumeier , Mikko Karttunen

Inspired by the formulation of quantum-electrodynamical time-dependent density functional theory (QED-TDDFT) by Rubio and coworkers, we propose an implementation that uses dimensionless amplitudes for describing the photonic contributions…

Materials Science · Physics 2021-08-20 Junjie Yang , Qi Ou , Zheng Pei , Hua Wang , Binbin Weng , Kieran Mullen , Yihan Shao

The practical success of density functional theory (DFT) is largely credited to the Kohn-Sham approach, which enables the exact calculation of the non-interacting electron kinetic energy via an auxiliary noninteracting system. Yet, the…

Computational Physics · Physics 2025-03-21 Sangita Majumdar , Zekun Shi , Giovanni Vignale

The Kohn-Sham approach to time-dependent density-functional theory (TDDFT) can be formulated, in principle exactly, by invoking the force-balance equation for the density, which leads to an explicit expression for the exchange-correlation…

Chemical Physics · Physics 2021-09-15 Walter Tarantino , Carsten A. Ullrich

In this contribution, we extend our framework for analyzing and visualizing correlated many-electron dynamics to non-variational, highly scalable electronic structure method. Specifically, an explicitly time-dependent electronic wave packet…

Chemical Physics · Physics 2017-04-27 Gunter Hermann , Vincent Pohl , Jean Christophe Tremblay

A direct orbital optimization method is presented for density functional calculations of excited electronic states using either a real space grid or a plane wave basis set. The method is variational, provides atomic forces in the excited…

Computational Physics · Physics 2022-11-09 Aleksei V. Ivanov , Gianluca Levi , Elvar Ö. Jónsson , Hannes Jónsson

Density functional theory (DFT) and linear-response time-dependent density functional theory (LR-TDDFT) rely on an exchange-correlation (xc) approximation that provides not only energy but also its functional derivatives that enter the…

Chemical Physics · Physics 2026-04-08 Xiaoyu Zhang

We formulate a time-dependent density functional theory (TDDFT) in terms of the density matrix to study ultrafast phenomena in semiconductor structures. A system of equations for the density matrix components, which is equivalent to the…

Mesoscale and Nanoscale Physics · Physics 2009-11-13 V. Turkowski , C. A. Ullrich

Development of the electronic kinetic-energy density functional is a subject of major interest in theoretical physics and chemistry. In this work, the nonlocal kinetic-energy functional is developed in terms of the response function for the…

Chemical Physics · Physics 2022-06-17 Hideaki Takahashi

Many-body theories such as dynamical mean field theory (DMFT) have enabled the description of the electron exchange-correlation interactions that are missing in current density functional theory (DFT) calculations. However, there has been…

Strongly Correlated Electrons · Physics 2021-01-19 A. D. N. James , E. I. Harris-Lee , A. Hampel , M. Aichhorn , S. B. Dugdale

Density functional theory (DFT) embedding provides a formally exact framework for interfacing correlated wave-function theory (WFT) methods with lower-level descriptions of electronic structure. Here, we report techniques to improve the…

Chemical Physics · Physics 2015-06-12 Jason D. Goodpaster , Taylor A. Barnes , Frederick R. Manby , Thomas F. Miller

We demonstrate for the first time that a functional-renormalization-group aided density-functional theory (FRG-DFT) describes well the characteristic features of the excited states as well as the ground state of an interacting many-body…

Nuclear Theory · Physics 2019-03-08 Takeru Yokota , Kenichi Yoshida , Teiji Kunihiro

The van Leeuwen proof of linear-response time-dependent density functional theory (TDDFT) is generalized to thermal ensembles. This allows generalization to finite temperatures of the Gross-Kohn relation, the exchange-correlation kernel of…

Chemical Physics · Physics 2016-06-15 Aurora Pribram-Jones , Paul E. Grabowski , Kieron Burke

Density functional theory has been an essential analysis tool for both theoretical and experimental chemists since accurate hybrid functionals were developed. Here we propose a local hybrid method derived from the optimized effective…

Chemical Physics · Physics 2017-03-24 Jaewook Kim , Kwangwoo Hong , Sang-Yeon Hwang , Seongok Ryu , Sunghwan Choi , Woo Youn Kim

Time-dependent density functional theory has emerged as a method of choice for calculations of spectra and response properties in physics, chemistry, and biology, with its system-size scaling enabling computations on systems much larger…

Chemical Physics · Physics 2021-07-13 Neepa T. Maitra

We investigate the behavior of oxygen vacancies in three different metal-oxide semiconductors (rutile and anatase TiO2, monoclinic WO3, and tetragonal ZrO2) using a recently proposed hybrid density-functional method in which the fraction of…

Density functional theory (DFT) has emerged as one of the most versatile and lucrative approaches in electronic structure calculations of many-electron systems in past four decades. Here we give an account of the development of a…

Chemical Physics · Physics 2019-04-19 Abhisek Ghosal , Amlan K. Roy

Linear-response time-dependent (TD) density-functional theory (DFT) has been implemented in the pseudopotential wavelet-based electronic structure program BigDFT and results are compared against those obtained with the all-electron…

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