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We describe an ab initio method for calculating the electronic structure, electronic transport, and forces acting on the atoms, for atomic scale systems connected to semi-infinite electrodes and with an applied voltage bias. Our method is…

Materials Science · Physics 2009-11-07 Mads Brandbyge , Jose-Luis Mozos , Pablo Ordejon , Jeremy Taylor , Kurt Stokbro

Systems whose underlying classical dynamics are chaotic exhibit signatures of the chaos in their quantum mechanics. We investigate the possibility of using time-dependent density functional theory (TDDFT) to study the case when chaos is…

Other Condensed Matter · Physics 2009-11-13 Adam Wasserman , Neepa T. Maitra , Eric J. Heller

This paper gives an introduction to the Keldysh formalism, with emphasis on its usefulness in time-dependent density functional theory. In the first part we introduce the Keldysh contour and the one-particle Green function defined on this…

Mesoscale and Nanoscale Physics · Physics 2007-05-23 Robert van Leeuwen , Nils Erik Dahlen , Gianluca Stefanucci , Carl-Olof Almbladh , Ulf von Barth

Orbital-free density functional theory (OF-DFT) provides an alternative approach for calculating the molecular electronic energy, relying solely on the electron density. In OF-DFT, both the ground-state density is optimized variationally to…

Chemical Physics · Physics 2023-11-23 Alexandre de Camargo , Ricky T. Q. Chen , Rodrigo A. Vargas-Hernández

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

Time-dependent density functional theory (TDDFT) is presently enjoying enormous popularity in quantum chemistry, as a useful tool for extracting electronic excited state energies. This article explains what TDDFT is, and how it differs from…

Materials Science · Physics 2007-05-23 Peter Elliott , Kieron Burke , Filipp Furche

Density functional theory (DFT) is the de facto approach for predicting self-consistent-field electronic structures of ground-state configurations of complex atoms, molecules, and solids and providing their property data for materials…

Materials Science · Physics 2024-01-30 Zi-Kui Liu

We show that the time dependent single electron, nuclear density matrix of an interacting electronic system coupled to nuclear degrees of freedom can be exactly reproduced by that of an electronic system with arbitrarily specified…

Materials Science · Physics 2009-02-07 Vinod Krishna

Orbital-optimized density functional theory (DFT) has emerged as an alternative to time-dependent (TD) DFT capable of describing difficult excited states with significant electron density redistribution, such as charge-transfer, Rydberg,…

Chemical Physics · Physics 2025-01-22 Hanh D. M. Pham , Rustam Z. Khaliullin

This paper develops a quantitatively accurate first-principles description for the frequency and the linewidth of collective electronic excitations in inhomogeneous weakly disordered systems. A finite linewidth in general has intrinsic and…

Mesoscale and Nanoscale Physics · Physics 2009-11-07 C. A. Ullrich , G. Vignale

Time-dependent density functional theory (TDDFT) is a standard approach for calculating optical excitations of molecules and solids, while ensemble DFT (EDFT) is a promising alternative under development. We introduce ensemble TDDFT…

Chemical Physics · Physics 2026-05-22 Kimberly J. Daas , Steven Crisostomo , Kieron Burke

Real-time time-dependent density functional theory (TDDFT) is presently the most accurate available method for computing electronic stopping powers from first principles. However, obtaining application-relevant results often involves either…

Materials Science · Physics 2023-07-10 Alina Kononov , Thomas Hentschel , Stephanie B. Hansen , Andrew D. Baczewski

Real-Time Time-Dependent Density Functional Theory (TDDFT) has become an attractive tool to model quantum dynamics on a first-principles Density Functional Theory level. In recent years, several developments and applications in this field…

Computational Physics · Physics 2020-08-21 Joscha Hekele , Peter Kratzer

Time-dependent density-functional theory (TDDFT) is a central tool for studying the dynamical electronic structure of molecules and solids, yet aspects of its mathematical foundations remain insufficiently understood. In this work, we…

We investigate the time an electronic excitation travels in a supermolecular setup using a measurement process in an open quantum-system framework. The approach is based on the stochastic Schr\"odinger equation and uses a Hamiltonian from…

Materials Science · Physics 2013-12-09 Dirk Hofmann , Heiko Appel , Massimiliano Di Ventra , Stephan Kümmel

First-order nonadiabatic coupling matrix elements (fo-NACMEs) are the basic quantities in theoretical descriptions of electronically nonadiabatic processes that are ubiquitous in molecular physics and chemistry. Given the large size of…

Chemical Physics · Physics 2021-05-25 Zikuan Wang , Chenyu Wu , Wenjian Liu

An exact theoretical framework based on Time Dependent Density Functional Theory (TDDFT) is proposed in order to deal with the time-dependent quantum transport in fully interacting systems. We use a \textit{partition-free} approach by Cini…

Mesoscale and Nanoscale Physics · Physics 2009-11-10 Gianluca Stefanucci , Carl-Olof Almbladh

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

Density functional theory (DFT) has greatly expanded our ability to affordably compute and understand electronic ground states, by replacing intractable {\em ab initio} calculations by models based on paradigmatic physics from high- and…

Chemical Physics · Physics 2023-03-29 Tim Gould , Derk P. Kooi , Paola Gori-Giorgi , Stefano Pittalis

Quantum Optimal Control Theory (QOCT) provides the necessary tools to theoretically design driving fields capable of controlling a quantum system towards a given state or along a prescribed path in Hilbert space. This theory must be…

Atomic and Molecular Clusters · Physics 2013-05-30 Alberto Castro , Jan Werschnik , Eberhard K. U. Gross