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The particle-hole interaction problem is longstanding within time-dependent density functional theory (TDDFT) and leads to extreme errors in the prediction of K-edge X-ray absorption spectra (XAS). We derive a linear-response formalism that…

Chemical Physics · Physics 2022-10-18 Kevin Carter-Fenk , Leonardo A. Cunha , Juan E. Arias-Martinez , Martin Head-Gordon

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

Single-particle methods based on Kohn-Sham unoccupied states to describe near-edge X-ray absorption (XAS) spectra are routinely applied for the description of K-edge spectra, as there is no complication due to spin-orbit (SO) coupling. L-…

Materials Science · Physics 2026-02-26 Esther A. B. Johnsen , Naoki Horiuchi , Toma Susi , Michael Walter

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

We present an implementation of time-dependent density-functional theory (TDDFT) in the linear response formalism enabling the calculation of low energy optical absorption spectra for large molecules and nanostructures. The method avoids…

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

We present a range-separated linear-response time-dependent density-functional theory (TDDFT) which combines a density-functional approximation for the short-range response kernel and a frequency-dependent second-order Bethe-Salpeter…

Chemical Physics · Physics 2016-03-23 Elisa Rebolini , Julien Toulouse

We prove the existence of the exact density-functional theory formalism for open electronic systems, and develop subsequently an exact time-dependent density-functional theory (TDDFT) formulation for the dynamic response. The TDDFT…

Chemical Physics · Physics 2007-05-23 Xiao Zheng , GuanHua Chen

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 present a new methodology for the linear-response time-dependent density functional theory (LR-TDDFT) calculation of the dynamic density response function of warm dense matter in an adiabatic approximation that can be used with any…

Computational Physics · Physics 2023-05-12 Zhandos A. Moldabekov , Michele Pavanello , Maximilian P. Boehme , Jan Vorberger , Tobias Dornheim

When running time-dependent density functional theory (TDDFT) calculations for real-time simulations of non-equilibrium dynamics, the user has a choice of initial Kohn-Sham state, and typically a Slater determinant is used. We explore the…

Chemical Physics · Physics 2016-08-24 Johanna I. Fuks , Soeren E. B. Nielsen , Michael Ruggenthaler , Neepa T. Maitra

We present a novel theoretical approach to simulate spin, time and angular-resolved photoelectron spectroscopy (ARPES) from first principles that is applicable to surfaces, thin films, few layer systems, and low-dimensional nanostructures.…

Computational Physics · Physics 2017-01-03 Umberto De Giovannini , Hannes Hübener , Angel Rubio

In ion irradiation processes, electronic stopping power describes the energy transfer rate from the irradiating ion to the target material's electrons. Due to the scarcity and significant uncertainties in experimental electronic stopping…

Materials Science · Physics 2018-05-04 Dillon C. Yost , Yi Yao , Yosuke Kanai

Time-dependent density functional theory (TDDFT) simulations of transient core-level spectroscopies require a balanced treatment of both valence- and core-electron excitations. To this end, tuned range-separated hybrid exchange-correlation…

Materials Science · Physics 2020-06-04 C. D. Pemmaraju

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

The adiabatic approximation in time-dependent density functional theory (TDDFT) is known to give an incorrect pole structure in the quadratic response function, leading to unphysical divergences in excited state-to-state transition…

Chemical Physics · Physics 2023-05-01 Davood Dar , Saswata Roy , Neepa T. Maitra

We study linear-response time-dependent density-functional theory (DFT) based on the single-determinant range-separated hybrid (RSH) scheme, i.e. combining a long-range Hartree-Fock exchange kernel with a short-range DFT…

Chemical Physics · Physics 2015-06-15 Elisa Rebolini , Andreas Savin , Julien Toulouse

Linear-response time-dependent Density Functional Theory (LR-TDDFT) is a widely used method for accurately predicting the excited-state properties of physical systems. Previous works have attempted to accelerate LR-TDDFT using heterogeneous…

Hardware Architecture · Computer Science 2025-04-07 Qingcai Jiang , Buxin Tu , Xiaoyu Hao , Junshi Chen , Hong An

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

A system of electrons in a local or nonlocal external potential can be studied with 1-matrix functional theory (1MFT), which is similar to density functional theory (DFT) but takes the one-particle reduced density matrix (1-matrix) instead…

Strongly Correlated Electrons · Physics 2008-07-23 Ryan Requist , Oleg Pankratov
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