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We propose a new method of calculating electronically excited states that combines a density functional theory (DFT) based ground state calculation with a linear response treatment that employs approximations used in the time-dependent…

Chemical Physics · Physics 2016-05-11 Robert Rüger , Erik van Lenthe , Thomas Heine , Lucas Visscher

The increasing need to simulate the dynamics of photoexcited molecular and nanosystems in the sub-picosecond regime demands new efficient tools able to describe the quantum nature of matter at a low computational cost. By combining the…

We present a new velocity-gauge real-time, time-dependent density functional tight-binding (VG-rtTDDFTB) implementation in the open-source DFTB+ software package (https://dftbplus.org) for probing electronic excitations in large, condensed…

Mesoscale and Nanoscale Physics · Physics 2024-05-24 Qiang Xu , Mauro Del Ben , Mahmut Sait Okyay , Min Choi , Khaled Z. Ibrahim , Bryan M. Wong

The time-dependent density functional based tight-binding (TD-DFTB) approach is generalized to account for fractional occupations. In addition, an on-site correction leads to marked qualitative and quantitative improvements over the…

Materials Science · Physics 2013-02-15 A. Domínguez , B. Aradi , T. Frauenheim , V. Lutsker , T. A. Niehaus

We have recently developed a method based on relativistic time-dependent density functional theory (TD-DFT) that allows the calculation of electronic spectra in solution (Creutzberg, Hedeg{\aa}rd, J. Chem. Theory Comput.18, 2022, 3671).…

Chemical Physics · Physics 2023-04-04 Joel Creutzberg , Erik Donovan Hedegård

Bridging the gap between first principles methods and empirical schemes, the density functional based tight-binding method (DFTB) has become a versatile tool in predictive atomistic simulations over the past years. One of the major…

Materials Science · Physics 2015-04-02 Vitalij Lutsker , Balint Aradi , Thomas A. Niehaus

Routine investigations of plasmonic phenomena at the quantum level present a formidable computational challenge due to the large system sizes and ultrafast timescales involved. This Feature Article highlights the use of density functional…

Mesoscale and Nanoscale Physics · Physics 2025-06-19 Nikhil S. Chellam , Subhajyoti Chaudhuri , Abhisek Ghosal , Sajal K. Giri , George C. Schatz

Under the Franck-Condon approximation, we systematically validated the performance of density functional theory (DFT) and the effects of anharmonicity in simulating C/N/O K-edge vibrationally-resolved X-ray spectra of common diatomic…

Chemical Physics · Physics 2025-01-06 Lu Zhang , Minrui Wei , Guoyan Ge , Weijie Hua

Following a previous paper [Y. Shi, Phys. Rev. C 98, 014329(2018)], we present an extension of the density-functional theory to allow for dynamic calculations based on the obtained static Hartree-Fock results. We perform extensive benchmark…

Nuclear Theory · Physics 2020-11-04 Yue Shi , Nobuo Hinohara , Bastian Schuetrumpf

During the last two decades density functional based linear response approaches have become the de facto standard for the calculation of optical properties of small and medium-sized molecules. At the heart of these methods is the solution…

Chemical Physics · Physics 2015-01-23 Robert Rüger , Erik van Lenthe , You Lu , Johannes Frenzel , Thomas Heine , Lucas Visscher

We investigate optical absorption spectra obtained through time-dependent density functional theory (TD-DFT) based on nonempirical hybrid functionals that are designed to correctly reproduce the dielectric function. The comparison with…

Materials Science · Physics 2020-08-17 Alexey Tal , Peitao Liu , Georg Kresse , Alfredo Pasquarello

Aluminum nanocrystals offer a promising platform for plasmonic photocatalysis, yet a detailed understanding of their electron dynamics and consequent photocatalytic performance has been challenging thus far due to computational limitations.…

Mesoscale and Nanoscale Physics · Physics 2025-04-29 Nikhil S. Chellam , George C. Schatz

We present background concepts of the nuclear density functional theory (DFT) and applications of the time-dependent DFT with the Skyrme energy functional for nuclear response functions. Practical methods for numerical applications of the…

Nuclear Theory · Physics 2013-10-16 T. Nakatsukasa , S. Ebata , P. Avogadro , L. Guo , T. Inakura , K. Yoshida

Optical properties of symmetry-forbidden pi-pi transitions in benzene are calculated with the time-dependent density functional theory (TDDFT), using an adiabatic LDA functional. Quantities calculated are the envelopes of the Franck-Condon…

Chemical Physics · Physics 2007-05-23 A. Schnell , G. F. Bertsch , K. Yabana

A generalization of the density-functional based tight-binding method (DFTB) for the use with range-separated exchange-correlation functionals is presented. It is based on the Generalized Kohn-Sham (GKS) formalism and employs the density…

Materials Science · Physics 2015-06-03 Thomas A. Niehaus , Fabio Della Sala

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

We present two improvements to the tight-binding approximation of time-dependent density functional theory (TD-DFTB): Firstly, we add an exact Hartree-Fock exchange term, which is switched on at large distances, to the ground state…

Chemical Physics · Physics 2015-10-28 Alexander Humeniuk , Roland Mitric

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

A derivation of non-adiabatic coupling vectors for the density functional based tight binding method (DFTB) between ground and excited states is presented. The analytical result is valid both for semi-local and long-range corrected DFTB and…

Chemical Physics · Physics 2020-10-29 Thomas A. Niehaus

Time-dependent density-functional theory (TDDFT) is a computationally efficient first-principles approach for calculating optical spectra in insulators and semiconductors, including excitonic effects. We show how exciton wave functions can…

Materials Science · Physics 2020-12-29 Jared R. Williams , Nicolas Tancogne-Dejean , Carsten A. Ullrich
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