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The particle-hole interaction problem is longstanding within time-dependent density functional theory (TDDFT) and leads to extreme errors in the prediction of K-edge X-ray absorption spectra (XAS). We derive a linear-response formalism that…

Chemical Physics · Physics 2022-10-18 Kevin Carter-Fenk , Leonardo A. Cunha , Juan E. Arias-Martinez , Martin Head-Gordon

The Kohn-Sham approach to time-dependent density-functional theory (TDDFT) can be formulated, in principle exactly, by invoking the force-balance equation for the density, which leads to an explicit expression for the exchange-correlation…

Chemical Physics · Physics 2021-09-15 Walter Tarantino , Carsten A. Ullrich

Recent advances in laser technology allow us to follow electronic motion at its natural time-scale with ultra-fast time resolution, leading the way towards attosecond physics experiments of extreme precision. In this work, we assess the use…

Other Condensed Matter · Physics 2016-06-22 Jessica Walkenhorst , Umberto De Giovannini , Alberto Castro , Angel Rubio

This paper introduces a spectral analysis of time-seires data derived from real-time time-dependent density functional theory (TDDFT) using Singular Spectrum Analysis (SSA). TDDFT is a robust method for obtaining molecular excited states…

Computational Physics · Physics 2025-10-02 Naoki Tani , Satoru S. Kano , Yasunari Zempo

An approximate solution to the time-dependent density functional theory (TDDFT) response equations for finite systems is developed, yielding corrections to the single-pole approximation. These explain why allowed Kohn-Sham transition…

Materials Science · Physics 2009-11-07 H. Appel , E. K. U. Gross , K. Burke

We present a time-dependent density functional theory (TDDFT) based approach to compute the light-matter couplings between two different manifolds of excited states relative to a common ground state. These quantities are the necessary…

By introducing the self-energy density functionals for the dissipative interactions between the reduced system and its environment, we develop a time-dependent density-functional theory formalism based on an equation of motion for the…

Quantum Physics · Physics 2009-11-13 Xiao Zheng , Fan Wang , Chi Yung Yam , Yan Mo , GuanHua Chen

The real-time electronic dynamics on material surfaces is critically important to a variety of applications. However, their simulations have remained challenging for conventional methods such as the time-dependent density-functional theory…

Chemical Physics · Physics 2015-06-16 Rulin Wang , Dong Hou , Xiao Zheng

Time-Dependent Density Functional Theory (TDDFT) has recently been extended to describe many-body open quantum systems (OQS) evolving under non-unitary dynamics according to a quantum master equation. In the master equation approach,…

Chemical Physics · Physics 2015-05-18 David G. Tempel , Mark A. Watson , Roberto Olivares-Amaya , Alán Aspuru-Guzik

We present the theory, implementation, and benchmarking of a real-time time-dependent density functional theory (RT-TDDFT) module within the RMG code, designed to simulate the electronic response of molecular systems to external…

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

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

We propose a machine learning based approach to develop the exchange-correlation potential of time dependent density functional theory (TDDFT). The neural network projection from the time-varying electron densities to the corresponding…

Computational Physics · Physics 2020-05-20 Yasumitsu Suzuki , Ryo Nagai , Jun Haruyama

Time-dependent density functional theory (TDDFT) is a widely used method to investigate electron dynamics under various external perturbations such as laser fields. In this work, we present a novel approach to accelerate real time TDDFT…

Materials Science · Physics 2024-07-29 Karan Shah , Attila Cangi

We demonstrate the capabilities of time-dependent density functional theory (TDDFT) for strong-field, short wavelength (soft X-ray) physics, as compared to a formalism based on rate equations. We find that TDDFT provides a very good…

We provide a new formulation of Time-Dependent Density Functional Theory (TDDFT) based on the geometric structure of the set of states constrained to have a fixed density. Orbital-free TDDFT is formulated using a hydrodynamics equation…

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

First principle theoretical modeling of out-of-equilibrium processes observed in attosecond pump-probe transient absorption spectroscopy (TAS) triggering pure electron dynamics remains a challenging task, specially for heavy elements and/or…

Chemical Physics · Physics 2023-02-14 Torsha Moitra , Lukas Konecny , Marius Kadek , Angel Rubio , Michal Repisky

Photo-active systems are characterized by their capacity of absorbing light energy and transforming it. Usually, more than one chromophore is involved in the light absorption and excitation transport processes in complex systems.…

Materials Science · Physics 2019-05-21 Joaquim Jornet-Somoza , Irina Lebedeva

When running time-dependent density functional theory (TDDFT) calculations for real-time simulations of non-equilibrium dynamics, the user has a choice of initial Kohn-Sham state, and typically a Slater determinant is used. We explore the…

Chemical Physics · Physics 2016-08-24 Johanna I. Fuks , Soeren E. B. Nielsen , Michael Ruggenthaler , Neepa T. Maitra