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Localized molecular orbitals are often used for the analysis of chemical bonds, but they can also serve to efficiently and comprehensibly compute linear response properties. While conventional canonical molecular orbitals provide an…

Chemical Physics · Physics 2023-02-08 Souloke Sen , Bruno Senjean , Lucas Visscher

Linear-response time-dependent Density Functional Theory (LR-TDDFT) is a widely used method for accurately predicting the excited-state properties of physical systems. Previous works have attempted to accelerate LR-TDDFT using heterogeneous…

Hardware Architecture · Computer Science 2025-04-07 Qingcai Jiang , Buxin Tu , Xiaoyu Hao , Junshi Chen , Hong An

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

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

The adiabatic approximation in time-dependent density functional theory (TDDFT) is known to give an incorrect pole structure in the quadratic response function, leading to unphysical divergences in excited state-to-state transition…

Chemical Physics · Physics 2023-05-01 Davood Dar , Saswata Roy , Neepa T. Maitra

The frequency-dependent response of a one-dimensional fermion system is investigated using Current Density Functional Theory (CDFT) within the local approximation (LDA). DFT-LDA, and in particular CDFT-LDA, reproduces very well the…

Strongly Correlated Electrons · Physics 2010-04-01 Michael Dzierzawa , Ulrich Eckern , Stefan Schenk , Peter Schwab

Subsystem Density-Functional Theory (DFT) is an emerging technique for calculating the electronic structure of complex molecular and condensed phase systems. In this topical review, we focus on some recent advances in this field related to…

Chemical Physics · Physics 2015-06-24 Alisa Krishtal , Debalina Sinha , Alessandro Genova , Michele Pavanello

The Quantum-Electrodynamical Time-Dependent Density Functional Theory (QED-TDDFT) equations are solved by time propagating the wave function on a tensor product of a Fock-space and real-space grid. Applications for molecules in cavities…

Quantum Physics · Physics 2022-11-30 Justin Malave , Alexander Ahrens , Daniel Pitagora , Cody Covington , Kálmán Varga

The general expectation that, in principle, time-dependent density functional theory (TDDFT) be an exact formulation of the time-evolution of an interacting N-electron system is critically reexamined. It is demonstrated that the previous…

Other Condensed Matter · Physics 2007-08-13 J. Schirmer , A. Dreuw

Time-dependent density-functional theory (TDDFT) often successfully reproduces excitation energies of finite systems, already in the adiabatic local-density approximation (ALDA). Here we show for prototypical molecular materials, i.e.,…

Materials Science · Physics 2015-11-25 Caterina Cocchi , Claudia Draxl

We discuss two problems which are particularly challenging for approximations in time-dependent density functional theory (TDDFT) to capture: momentum-distributions in ionization processes, and memory-dependence in real-time dynamics. We…

Materials Science · Physics 2010-03-22 Arun K. Rajam , Paul Hessler , Christian Gaun , Neepa T. Maitra

Ab initio modeling of dynamic structure factors (DSF) and related density response properties in the warm dense matter (WDM) regime is a challenging computational task. The DSF, convolved with a probing X-ray beam and instrument function,…

We report on a general method for the calculation of the frequency-dependent optical response of clusters based upon time-dependent density functional theory (TDDFT). The implementation is done using explicit propagation in the time domain…

Materials Science · Physics 2009-11-07 Argyrios Tsolakidis , Daniel Sanchez-Portal , Richard M. Martin

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

We present the extension of Frozen Density Embedding (FDE) theory to real-time Time Dependent Density Functional Theory (rt-TDDFT). FDE a is DFT-in-DFT embedding method that allows to partition a larger Kohn-Sham system into a set of…

Chemical Physics · Physics 2015-06-23 Alisa Krishtal , Davide Ceresoli , Michele Pavanello

Local density approximation (LDA) to the density functional theory (DFT) has continuous derivative of total energy as a number of electrons function and continuous exchange-correlation potential, while in exact DFT both should be…

Strongly Correlated Electrons · Physics 2010-06-28 V. I. Anisimov , A. V. Kozhevnikov , M. A. Korotin , A. V. Lukoyanov , D. A. Khafizullin

We analyze possible nonlinear exciton-exciton correlation effects in the optical response of semiconductors by using a time-dependent density-functional theory (TDDFT) approach. For this purpose, we derive the nonlinear (third-order) TDDFT…

Materials Science · Physics 2015-06-16 Volodymyr Turkowski , Michael N. Leuenberger

Multipole moments are the first order responses of the energy to spatial derivatives of the electric field strength. The quality of density functional theory (DFT) prediction of molecular multipole moments thus characterizes errors in…

Chemical Physics · Physics 2021-02-23 Diptarka Hait , Yu Hsuan Liang , Martin Head-Gordon

The 2p-3d core hole interaction in the L2,3 absorption spectra of the 3d transition metals is treated within time-dependent density functional theory (TDDFT). A simple three-level model explains the origin of the strong deviations from the…

Materials Science · Physics 2009-11-11 A. Scherz , E. K. U. Gross , H. Appel , C. Sorg , K. Baberschke , H. Wende , K. Burke

X-ray Thomson scattering (XRTS) constitutes an essential technique for diagnosing material properties under extreme conditions, such as high pressures and intense laser heating. Time-dependent density functional theory (TDDFT) is one of the…