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DFT calculations have become widespread in both chemistry and materials, because they usually provide useful accuracy at much lower computational cost than wavefunction-based methods. All practical DFT calculations require an approximation…

Chemical Physics · Physics 2022-03-15 Eunji Sim , Suhwan Song , Stefan Vuckovic , Kieron Burke

We present a numerical modeling workflow based on machine learning (ML) which reproduces the the total energies produced by Kohn-Sham density functional theory (DFT) at finite electronic temperature to within chemical accuracy at negligible…

We propose a computationally efficient approach to the nonadiabatic time-dependent density functional theory (TDDFT) which is based on a representation of the frequency-dependent exchange correlation kernel as a response of a set of damped…

Mesoscale and Nanoscale Physics · Physics 2019-12-18 Dmitry R. Gulevich , Yaroslav V. Zhumagulov , Alexei V. Vagov , Vasili Perebeinos

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 solution of the full TDDFT eigenvalue equation in the linear response formalism exhibiting a linear-scaling computational complexity with system size, without relying on the simplifying Tamm-Dancoff approximation (TDA). The…

Computational Physics · Physics 2016-01-20 Tim J. Zuehlsdorff , Nicholas D. M. Hine , Mike C. Payne , Peter D. Haynes

Time-dependent density-functional theory (TDDFT) is a computationally efficient first-principles approach for calculating optical spectra in insulators and semiconductors, including excitonic effects. We show how exciton wave functions can…

Materials Science · Physics 2020-12-29 Jared R. Williams , Nicolas Tancogne-Dejean , Carsten A. Ullrich

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

The derivative discontinuity of the exchange-correlation (xc) energy at integer particle number is a property of the exact, unknown xc functional of density functional theory (DFT) which is absent in many popular local and semilocal…

Strongly Correlated Electrons · Physics 2015-06-11 Gao Xianlong , A-Hai Chen , I. V. Tokatly , S. Kurth

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 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

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

The real-time-propagation formulation of time-dependent density-functional theory (RT-TDDFT) is an efficient method for modeling the optical response of molecules and nanoparticles. Compared to the widely adopted linear-response TDDFT…

Materials Science · Physics 2019-01-15 Tuomas P. Rossi , Mikael Kuisma , Martti J. Puska , Risto M. Nieminen , Paul Erhart

Due to its favorable computational efficiency time-dependent (TD) density functional theory (DFT) enables the prediction of electronic spectra in a high-throughput manner across chemical space. Its predictions, however, can be quite…

Energy transfer processes from a high-intensity ultrashort laser pulse to electrons in simple dielectrics, silicon, diamond, and $\alpha$-quartz are theoretically investigated by first-principles calculations based on time-dependent density…

Optics · Physics 2019-05-22 Atsushi Yamada , Kazuhiro Yabana

We introduce 'single-particle-exact density functional theory' (1pEx-DFT), a novel density functional approach that represents all single-particle contributions to the energy with exact functionals. Here, we parameterize interaction energy…

The systematic underestimation of band gaps is one of the most fundamental challenges in semilocal density functional theory (DFT). In addition to hindering the application of DFT to predicting electronic properties, the band gap problem is…

Chemical Physics · Physics 2024-08-27 Kyle Bystrom , Stefano Falletta , Boris Kozinsky

The key features of density-functional theory (DFT) within a minimalistic implementation of quantum electrodynamics are demonstrated, thus allowing to study elementary properties of quantum-electrodynamical density-functional theory…

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

Linear-response quantum electrodynamical density functional theory (QEDFT) enables the description of molecular spectra under strong coupling to quantized photonic modes, such as those in optical cavities. Recently, this approach was…

Chemical Physics · Physics 2025-07-11 Lukas Konecny , Valeriia P. Kosheleva , Michael Ruggenthaler , Michal Repisky , Angel Rubio

We train a neural network as the universal exchange-correlation functional of density-functional theory that simultaneously reproduces both the exact exchange-correlation energy and potential. This functional is extremely non-local, but…

Computational Physics · Physics 2019-10-10 Jonathan Schmidt , Carlos L. Benavides-Riveros , Miguel A. L. Marques