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Quantum--Mechanical methods that are both computationally fast and accurate are not yet available for electronic excitations having charge transfer character. In this work, we present a significant step forward towards this goal for those…

Chemical Physics · Physics 2015-06-12 Michele Pavanello , Troy Van Voorhis , Lucas Visscher , Johannes Neugebauer

Spectroscopies that probe electronic excitations from core levels into unoccupied orbitals, such as X-ray absorption spectroscopy and electron energy loss spectroscopy, are widely used to gain insight into the electronic and chemical…

Materials Science · Physics 2022-09-12 Marcus Annegarn , Juhan Matthias Kahk , Johannes Lischner

Almost all time-dependent density-functional theory (TDDFT) calculations of excited states make use of the adiabatic approximation, which implies a frequency-independent exchange-correlation kernel that limits applications to…

Mesoscale and Nanoscale Physics · Physics 2011-12-08 Miquel Huix-Rotllant , Andrei Ipatov , Angel Rubio , Mark E. Casida

We consider the calculations of photoionization spectra and core resonances of open-shell systems using range-separated time-dependent density-functional theory. Specifically, we use the time-dependent range-separated hybrid (TDRSH) scheme,…

Chemical Physics · Physics 2023-01-11 Julien Toulouse , Karno Schwinn , Felipe Zapata , Antoine Levitt , Eric Cancès , Eleonora Luppi

Time-dependent density-functional theory (TDDFT) is widely used to describe electronic excitations in complex finite systems with large numbers of atoms, such as biomolecules and nanocrystals. The first part of this paper will give a simple…

Materials Science · Physics 2008-08-15 C. A. Ullrich , V. Turkowski

Density functional theory (DFT) offers a desirable balance between quantitative accuracy and computational efficiency in practical many-electron calculations. Its central component, the exchange-correlation energy functional, has been…

Recent progress in the field of (time-independent) ensemble density-functional theory (DFT) for excited states are reviewed. Both Gross-Oliveira-Kohn (GOK) and $N$-centered ensemble formalisms, which are mathematically very similar and…

Chemical Physics · Physics 2021-11-29 Filip Cernatic , Bruno Senjean , Vincent Robert , Emmanuel Fromager

Perdew et al. [Phys. Rev. Lett 49, 1691 (1982)] discovered and proved two different properties of exact Kohn-Sham density functional theory (DFT): (i) The exact total energy versus particle number is a series of linear segments between…

Other Condensed Matter · Physics 2015-03-13 Tamar Stein , Jochen Autschbach , Niranjan Govind , Leeor Kronik , Roi Baer

A very specific ensemble of ground and excited states is shown to yield an exact formula for any excitation energy as a simple correction to the energy difference between orbitals of the Kohn-Sham ground state. This alternative scheme…

Chemical Physics · Physics 2017-07-26 Zeng-hui Yang , Aurora Pribram-Jones , Kieron Burke , Carsten A. Ullrich

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

The most accurate theoretical method to describe excitons is the solution of the Bethe-Salpeter equation in the GW approximation (GW-BSE). However, because of its computation cost, time-dependent density functional theory (TDDFT) is…

Materials Science · Physics 2023-01-11 Rita Maji , Elena Degoli , Monica Calatayud , Valérie Véniard , Eleonora Luppi

Time dependent quantum systems are the subject of intense inquiry, in mathematics, science, and engineering, particularly at the atomic and molecular levels. In 1984, Runge and Gross introduced time dependent density functional theory…

Analysis of PDEs · Mathematics 2021-02-24 Joseph W. Jerome

We investigate the time an electronic excitation travels in a supermolecular setup using a measurement process in an open quantum-system framework. The approach is based on the stochastic Schr\"odinger equation and uses a Hamiltonian from…

Materials Science · Physics 2013-12-09 Dirk Hofmann , Heiko Appel , Massimiliano Di Ventra , Stephan Kümmel

We develop an efficient approach to evaluate range-separated exact exchange for grid or plane-wave based representations within the Generalized Kohn-Sham DFT (GKS-DFT) framework. The Coulomb kernel is fragmented in reciprocal space, and we…

Chemical Physics · Physics 2023-09-11 Nadine C. Bradbury , Tucker Allen , Minh Nguyen , Daniel Neuhauser

Static electric response properties of atoms and molecules are reported within the real-space Cartesian grid implementation of pseudopotential Kohn-Sham (KS) density functional theory (DFT). A detailed systematic investigation is made for a…

Chemical Physics · Physics 2019-04-26 Tanmay Mandal , Abhisek Ghosal , Amlan K. Roy

Ensemble density-functional theory (eDFT) suffers from the so-called "ghost interaction" error when approximate exchange-correlation functionals are used. In this work, we present a rigorous ghost interaction correction (GIC) scheme in the…

Chemical Physics · Physics 2016-07-21 Md. Mehboob Alam , Stefan Knecht , Emmanuel Fromager

In order to obtain a reasonably accurate and easily implemented approach to many-electron calculations, we will develop a new Density Functional Theory (DFT). Specifically, we derive an approximation to electron density, the first term of…

Materials Science · Physics 2010-04-23 Gregory C. Dente

Efficiently recovering dynamic correlation in strongly correlated systems without incurring prohibitive computational costs remains a central challenge in quantum chemistry. In this Perspective, we review and benchmark methods capable of…

Chemical Physics · Physics 2026-05-22 Michał Hapka , Aleksandra Tucholska , Katarzyna Pernal

Density functional theory (DFT) has greatly expanded our ability to affordably compute and understand electronic ground states, by replacing intractable {\em ab initio} calculations by models based on paradigmatic physics from high- and…

Chemical Physics · Physics 2023-03-29 Tim Gould , Derk P. Kooi , Paola Gori-Giorgi , Stefano Pittalis

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