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We present an efficient method for propagating the time-dependent Kohn-Sham equations in free space, based on the recently introduced Fourier contour deformation (FCD) approach. For potentials which are constant outside a bounded domain,…

Chemical Physics · Physics 2023-07-10 Jason Kaye , Alex Barnett , Leslie Greengard , Umberto De Giovannini , Angel Rubio

We revisit Kohn-Sham time-dependent density-functional theory (TDDFT) equations and show that they derive from a canonical Hamiltonian formalism. We use this geometric description of the TDDFT dynamics to define families of symplectic…

Computational Physics · Physics 2023-11-20 Francois Mauger , Cristel Chandre , Mette B. Gaarde , Kenneth Lopata , Kenneth J. Schafer

While quantum computers have shown significant promise for electronic structure calculations, their potential to accelerate density functional theory (DFT) calculations remains unclear. In this work, we present a qubit-efficient encoding…

Exact (Hartree Fock) exchange is needed to overcome some of the limitations of local and semilocal approximations of density functional theory (DFT). So far, however, computational cost has limited the use of exact exchange in plane wave…

Strongly Correlated Electrons · Physics 2009-11-13 Xifan Wu , Annabella Selloni , Roberto Car

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…

While in principle exact, Kohn-Sham density functional theory -- the workhorse of computational chemistry -- must rely on approximations for the exchange-correlation functional. Despite staggering successes, present-day approximations still…

Aiming to combine density functional theory (DFT) and wavefunction theory, we study a mapping from the many-body interacting system to an effectively-interacting Kohn-Sham system instead of a non-interacting Kohn-Sham system. Because a…

Chemical Physics · Physics 2020-02-19 Shunsuke A. Sato , Angel Rubio

This article is part-I of a review of density-functional theory (DFT) that is the most widely used method for calculating electronic structure of materials. The accuracy and ease of numerical implementation of DFT methods has resulted in…

Materials Science · Physics 2023-05-25 Prashant Singh , Manoj K Harbola

We have developed and implemented a new quantum molecular dynamics approximation that allows fast and accurate simulations of dense plasmas from cold to hot conditions. The method is based on a carefully designed orbital-free implementation…

Plasma Physics · Physics 2015-06-22 Travis Sjostrom , Jerome Daligault

Screened range-separated hybrid (SRSH) functionals within generalized Kohn-Sham density functional theory (GKS-DFT) have been shown to restore a general $1/(r\varepsilon)$ asymptotic decay of the electrostatic interaction in dielectric…

Computational Physics · Physics 2023-06-26 Tammo van der Heide , Bálint Aradi , Ben Hourahine , Thomas Frauenheim , Thomas A. Niehaus

Density Functional Theory (DFT) is a pivotal method within quantum chemistry and materials science, with its core involving the construction and solution of the Kohn-Sham Hamiltonian. Despite its importance, the application of DFT is…

The marriage of density functional theory (DFT) and deep learning methods has the potential to revolutionize modern computational materials science. Here we develop a deep neural network approach to represent DFT Hamiltonian (DeepH) of…

Materials Science · Physics 2023-01-02 He Li , Zun Wang , Nianlong Zou , Meng Ye , Runzhang Xu , Xiaoxun Gong , Wenhui Duan , Yong Xu

Orbital-free density functional theory (OF-DFT) constitutes a computationally highly effective tool for modeling electronic structures of systems ranging from room-temperature materials to warm dense matter. Its accuracy critically depends…

The combination of density functional theory with dynamical mean-field theory (DFT+DMFT) has become a powerful first-principles approach to tackle strongly correlated materials in condensed matter physics. The wide use of this approach…

Strongly Correlated Electrons · Physics 2022-05-10 Xin Qu , Peng Xu , Rusong Li , Gang Li , Lixin He , Xinguo Ren

Kohn-Sham density functional theory is the base of modern computational approaches to electronic structures. Their accuracy vitally relies on the exchange-correlation energy functional, which encapsulates electron-electron interaction…

Computational Physics · Physics 2019-11-04 Ryo Nagai , Ryosuke Akashi , Osamu Sugino

The widely-used Kohn-Sham implementation of density functional theory (DFT) maps a system of interacting electrons onto an auxiliary non-interacting one and is presumably inaccurate for strongly correlated materials. We present a concrete…

Strongly Correlated Electrons · Physics 2024-05-31 Jamin Kidd , Ruiqi Zhang , Shao-Kai Jian , Jianwei Sun

We propose a local real-space formulation for orbital-free DFT with density dependent kinetic energy functionals and a unified variational framework for computing the configurational forces associated with geometry optimization of both…

Materials Science · Physics 2015-06-15 Sambit Das , Mrinal Iyer , Vikram Gavini

This work presents an alternative, general, and in-principle exact extension of electronic Kohn-Sham density functional theory (KS-DFT) to the fully quantum-mechanical molecular problem. Unlike in existing multi-component or…

Chemical Physics · Physics 2024-05-14 Emmanuel Fromager , Benjamin Lasorne

Spin-current density functional theory (SCDFT) is a formally exact framework designed to handle the treatment of interacting many-electron systems including spin-orbit coupling at the level of the Pauli equation. In practice, robust and…

Real-time time-dependent density functional theory (RT-TDDFT) is a powerful approach for investigating various ultrafast phenomena in materials. However, most existing RT-TDDFT studies rely on adiabatic local or semi-local approximations,…

Materials Science · Physics 2025-12-23 Yuyang Ji , Haotian Zhao , Peize Lin , Xinguo Ren , Lixin He