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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

In this paper we demonstrate the performance of several density-based methods in predicting the inversion of S$_1$ and T$_1$ states of a few N-heterocyclic fused ring molecules (popularly known as INVEST molecules) with an eye to identify a…

Chemical Physics · Physics 2024-08-12 Shamik Chanda , Subhasish Saha , Sangita Sen

The design of better exchange-correlation functionals for Density Functional Theory (DFT) is a central challenge of modern electronic structure theory. However, current developments are limited by the mathematical form of the functional,…

Chemical Physics · Physics 2024-08-19 Kyle Bystrom , Boris Kozinsky

The present work proposes an approach to obtain a basis-set correction based on density-functional theory (DFT) for the computation of molecular properties in wave-function theory (WFT). This approach allows one to accelerate the basis-set…

Chemical Physics · Physics 2022-05-18 Diata Traore , Julien Toulouse , Emmanuel Giner

Using a linear combination of atomic orbitals approach, we report a systematic comparison of various Density Functional Theory (DFT) and hybrid exchange-correlation functionals for the prediction of the electronic and structural properties…

Materials Science · Physics 2008-05-07 D. I. Bilc , R. Orlando , R. Shaltaf , G. -M. Rignanese , Jorge Íñiguez , Ph. Ghosez

In the framework of DFT, the lowest triplet excited state, T$_1$, can be evaluated using multiple formulations, the most straightforward of which are UDFT and TDDFT. Assuming the exact XC functional is applied, UDFT and TDDFT provide…

Chemical Physics · Physics 2019-01-17 Zhou Lin , Troy Van Voorhis

The accurate prediction of singlet and triplet excitation energies is of significant fundamental interest and is critical for many applications. An area of intense research, most calculations of singlet and triplet energies use…

Computational Physics · Physics 2017-05-22 Tonatiuh Rangel , Samia M. Hamed , Fabien Bruneval , Jeffrey B. Neaton

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

We compare two different approaches to investigations of many-electron systems. The first is the Hartree-Fock (HF) method and the second is the Density Functional Theory (DFT). Overview of the main features and peculiar properties of the HF…

Materials Science · Physics 2009-11-07 M. Ya. Amusia , A. Z. Msezane , V. R. Shaginyan

Time-dependent density functional theory (TDDFT) within the linear response regime provides a solid mathematical framework to capture excitations. The accuracy of the theory, however, largely depends on the approximations for the…

Strongly Correlated Electrons · Physics 2023-11-01 Aaron D. Kaplan , Adrienn Ruzsinszky

We present an \emph{Effective Static Approximation} (ESA) to the local field correction (LFC) of the electron gas that enables highly accurate calculations of electronic properties like the dynamic structure factor $S(q,\omega)$, the static…

Some of the most spectacular failures of density-functional and Hartree-Fock theories are related to an incorrect description of the so-called static electron correlation. Motivated by recent progress on the N-representability problem of…

We propose a new method of calculating electronically excited states that combines a density functional theory (DFT) based ground state calculation with a linear response treatment that employs approximations used in the time-dependent…

Chemical Physics · Physics 2016-05-11 Robert Rüger , Erik van Lenthe , Thomas Heine , Lucas Visscher

To examine the applicability of the time-dependent density-functional theory (TDDFT) for treating the electron-nucleus coupling in excited states, we calculate the strength distribution associated with the pi-pi* transition in ethylene. The…

Chemical Physics · Physics 2007-05-23 G. F. Bertsch , J. Giansiracusa , K. Yabana

Time-dependent density-functional theory (TDDFT) is a powerful tool to study the non-equilibrium dynamics of inhomogeneous interacting many-body systems. Here we show that the simple adiabatic local-spin-density approximation for the…

Strongly Correlated Electrons · Physics 2008-11-11 Wei Li , Gao Xianlong , Corinna Kollath , Marco Polini

Following a recent work [E. Fromager, J. Phys. Chem. A 2025, 129, 4, 1143-1155] on the ensemble density functional theory (DFT) of excited electronic energy levels, we derive in this paper the ensuing static linear response theory, thus…

Chemical Physics · Physics 2025-09-26 Lucien Dupuy , Emmanuel Fromager

We extend our recently developed sparse-stochastic fragmented exchange formalism for ground-state hybrid DFT (ngH-DFT) to calculate absorption spectra within linear-response time-dependent Generalized Kohn-Sham DFT (LR-GKS-TDDFT), for…

Chemical Physics · Physics 2025-03-11 Mykola Sereda , Tucker Allen , Nadine C. Bradbury , Khaled Z. Ibrahim , Daniel Neuhauser

Density functional theory (DFT) remains the most widely used electronic structure method. Although exact in principle, in practice, it relies on approximations to the exchange-correlation (XC) functional, which is known to be a unique…

Computational Physics · Physics 2025-10-14 Vishal Subramanian , Bikash Kanungo , Vikram Gavini

A simple approximate solution to the linear response equations of time-dependent density functional theory (TDDFT) is given. This extends the single-pole approximation (SPA) to two strongly-coupled poles. The analysis provides both an…

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

A review of the approximations in any time-dependent density functional calculation of excitation energies is given. The single-pole approximation for the susceptibility is used to understand errors in popular approximations for the…

Materials Science · Physics 2007-05-23 Kieron Burke , Martin Petersilka , E. K. U. Gross