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We present a new class of non-adiabatic approximations in time-dependent density functional theory derived from an exact expression for the time-dependent exchange-correlation potential. The approximations reproduce dynamical step and peak…

Chemical Physics · Physics 2018-12-21 Lionel Lacombe , Neepa T. Maitra

Density functional theory with linear combination of atomic orbitals (LCAO) basis sets is useful for studying large atomic systems, especially when it comes to computationally highly demanding time-dependent dynamics. We have implemented…

Materials Science · Physics 2025-05-02 Vladimír Zobač , Mikael Kuisma , Ask Hjorth Larsen , Tuomas Rossi , Toma Susi

To leverage the redundancy between the electronic structure computed at each step of first-principles molecular dynamics, we present a data-driven modeling framework for Kohn-Sham Density Functional Theory that bypasses the explicit…

Numerical Analysis · Mathematics 2026-02-27 Siu Wun Cheung , Youngsoo Choi , Jean-Luc Fattebert , Jonas Kaufman , Daniel Osei-Kuffuor

Time-dependent density functional theory is extended to include dissipative systems evolving under a master equation, providing a Hamiltonian treatment for molecular electronics. For weak electric fields, the isothermal conductivity is…

Materials Science · Physics 2007-05-23 Kieron Burke , Roberto Car , Ralph Gebauer

In the current density functional theory of linear and nonlinear time-dependent phenomena, the treatment of exchange and correlation beyond the level of the adiabatic local density approximation is shown to lead to the appearance of…

Condensed Matter · Physics 2009-10-30 G. Vignale , C. A. Ullrich , S. Conti

An economic modeling approach for cavity quantum electrodynamics is provided by mean-field dynamics, wherein the optical field is described classically while a self-consistent interaction with quantum emitters is incorporated through the…

Chemical Physics · Physics 2025-12-10 Ming-Hsiu Hsieh , Alex Krotz , Roel Tempelaar

Electron-positron interactions have been utilized in various fields of science. Here we develop time-dependent multi-component density functional theory to study the coupled electron-positron dynamics from first principles. We prove that…

Chemical Physics · Physics 2018-10-03 Yasumitsu Suzuki , Satoshi Hagiwara , Kazuyuki Watanabe

A practical computational scheme based on time-dependent density functional theory (TDDFT) and ultrasoft pseudopotential (USPP) is developed to study electron dynamics in real time. A modified Crank-Nicolson time-stepping algorithm is…

Materials Science · Physics 2007-05-23 Xiaofeng Qian , Ju Li , Xi Lin , Sidney Yip

Imaginary-time time-dependent Density functional theory (it-TDDFT) has been proposed as an alternative method for obtaining the ground state within density functional theory (DFT) which avoids some of the difficulties with convergence…

Computational Physics · Physics 2021-11-09 John McFarland , Efstratios Manousakis

A decomposition of the exact exchange-correlation potential of time-dependent density functional theory into an interaction component and a kinetic component offers a new starting point for non- adiabatic approximations. The components are…

Chemical Physics · Physics 2018-11-14 Johanna I. Fuks , Lionel Lacombe , Soeren E. B. Nielsen , Neepa T. Maitra

We present a simple geometrical "fluidic" approximation to the non-adiabatic part of the Kohn-Sham potential, $v_{\mathrm{KS}}$, of time-dependent density functional theory. This part of $v_{\mathrm{KS}}$ is often crucial, but most…

Chemical Physics · Physics 2020-03-25 Mike Entwistle , Rex Godby

Two electrons at the threshold of ionization represent a severe test case for electronic structure theory. A pseudospectral method yields a very accurate density of the two-electron ion with nuclear charge close to the critical value.…

Chemical Physics · Physics 2014-08-12 Paul E. Grabowski , Kieron Burke

The exact ground-state exchange-correlation functional of Kohn-Sham density functional theory yields the exact transmission through an Anderson junction at zero bias and temperature. The exact impurity charge susceptibility is used to…

Mesoscale and Nanoscale Physics · Physics 2015-06-03 Zhenfei Liu , Justin P. Bergfield , Kieron Burke , Charles A. Stafford

The simplest density functional theory due to Thomas, Fermi, Dirac and Weizsacker is employed to describe the non-equilibrium thermodynamic evolution of an electron gas. The temperature effect is introduced via the Fermi-Dirac entropy,…

Quantum Physics · Physics 2015-06-25 R. Tsekov

Nuclear quantum effects and non-Born--Oppenheimer effects play a vital role in many chemical and biological processes, motivating the incorporation of such effects into dynamical simulations. In real-time nuclear--electronic orbital…

Chemical Physics · Physics 2026-05-27 Nicholas J. Boyer , Sharon Hammes-Schiffer

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

Mixed quantum-classical mechanics descriptions are critical to modeling coupled electron-nuclear dynamics, i.e. non-adiabatic molecular dynamics, relevant to photochemical and photophysical processes. We argue that, for polyatomic…

Chemical Physics · Physics 2018-08-21 Roman Baskov , Alexander White , Dmitry Mozyrsky

We show that an asymmetric two-fermion two-site Hubbard model illustrates the essential features of long-range charge-transfer dynamics in a real-space molecule. We apply a resonant field that transfers one fermion from one site to the…

Chemical Physics · Physics 2015-06-18 J. I. Fuks , N. T. Maitra

A first-principles approach to describe electron dynamics in open quantum systems driven far from equilibrium via external time-dependent stimuli is introduced. Within this approach, the driven Liouville von Neumann methodology is used to…

Mesoscale and Nanoscale Physics · Physics 2023-05-10 Annabelle Oz , Abraham Nitzan , Oded Hod , Juan E. Peralta

Last year, at least 30,000 scientific papers used the Kohn-Sham scheme of density functional theory to solve electronic structure problems in a wide variety of scientific fields, ranging from materials science to biochemistry to…

Computational Physics · Physics 2018-02-07 Felix Brockherde , Leslie Vogt , Li Li , Mark E. Tuckerman , Kieron Burke , Klaus-Robert Müller
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