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We establish time-resolved high harmonic generation (tr-HHG) as a powerful spectroscopy for photoinduced dynamics in strongly correlated materials through a detailed investigation of the insulator-to-metal transitions in vanadium dioxide.…

Molecular absorption and photo-electron spectra can be efficiently predicted with real-time time-dependent density-functional theory (TDDFT). We show here how these techniques can be easily extended to study time-resolved pump-probe…

Atomic and Molecular Clusters · Physics 2013-01-10 Umberto De Giovannini , Gustavo Brunetto , Alberto Castro , Jessica Walkenhorst , Angel Rubio

Time-dependent density functional theory is widely used to describe excitations of many-fermion systems. In its many applications, 3D coordinate-space representation is used, and infinite-domain calculations are limited to a finite volume…

Nuclear Theory · Physics 2016-05-11 B. Schuetrumpf , W. Nazarewicz , P. -G. Reinhard

An atomic-orbital basis set framework is presented for carrying out velocity- gauge real-time time-dependent density functional theory (TDDFT) simulations in periodic systems employing range-separated hybrid functionals. Linear optical…

Materials Science · Physics 2018-10-02 C. D. Pemmaraju

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

Rabi oscillations have long been thought to be out of reach in simulations using time-dependent density functional theory (TDDFT), a prominent symptom of the failure of the adiabatic approximation for non-perturbative dynamics. We present a…

Chemical Physics · Physics 2024-06-21 Davood B. Dar , Anna Baranova , Neepa T. Maitra

Optical processes in insulators and semiconductors, including excitonic effects, can be described in principle exactly using time-dependent density-functional theory (TDDFT). Starting from a linearization of the TDDFT semiconductor Bloch…

Materials Science · Physics 2015-05-13 V. Turkowski , C. A. Ullrich

We present ultra-fast quantum chemical methods for the calculation of infrared and ultraviolet-visible spectra designed to provide fingerprint information during autonomous and interactive explorations of molecular structures.…

Chemical Physics · Physics 2022-08-30 Francesco Bosia , Thomas Weymuth , Markus Reiher

The atomistic resolution recently achieved by ultrafast spectroscopies demands corresponding theoretical advances. Real-time time-dependent density-functional theory (RT-TDDFT) with Ehrenfest dynamics offers an optimal trade-off between…

Materials Science · Physics 2022-10-19 Jannis Krumland , Matheus Jacobs , Caterina Cocchi

Nuclear inelastic scattering in conjunction with density functional theory (DFT) calculations has been applied for the identification of vibrational modes of the high-spin ferric and the high-spin ferrous iron-sulfur center of a…

We show that time-dependent density functional theory (TDDFT) is applicable to coherent optical phonon generation by intense laser pulses in solids. The two mechanisms invoked in phenomenological theories, namely impulsively stimulated…

Materials Science · Physics 2010-06-22 Y. Shinohara , Y. Kawashita , K. Yabana , J. -I. Iwata , T. Obote , G. F. Bertsch

We study formation of the Vibrational Distribution Function (VDF) in a molecular gas at low pressure, when vibrational levels are excited by electron impact and deactivated in collisions with walls and show that this problem has a…

Plasma Physics · Physics 2019-11-13 Wei Yang , Alexander V. Khrabrov , Igor D. Kaganovich , You-Nian Wang

Two difficulties associated with the computations of thermal vibrational correlation functions are discussed. The first one is the lack of a well-behaved expression that is valid at both high-temperature and $T \to 0$ K limits.…

Chemical Physics · Physics 2022-06-22 Rami Gherib , Scott N. Genin , Ilya G. Ryabinkin

Within the framework of ab initio time-dependent density-functional theory (TD-DFT), we propose a static approximation to the exchange-correlation kernel based on the jellium-with-gap model. This kernel accounts for electron-hole…

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

Time-Dependent Density Functional Theory (TDDFT) has been currently established as a computationally cheaper, yet effective, alternative to the Many-Body Perturbation Theory (MBPT) for calculating the optical properties of solids. Within…

Materials Science · Physics 2026-04-13 M. Arruabarrena , A. Leonardo , A. Ayuela

A numerical method to integrate the time-dependent Hartree-Fock Bogoliubov (TDHFB) equations with Gogny interaction is proposed. The feasibility of the TDHFB code is illustrated by the conservation of the energy, particle numbers, and…

Nuclear Theory · Physics 2015-06-04 Yukio Hashimoto

Density functional theory (DFT) provides a theoretical framework for efficient and fairly accurate calculations of the electronic structure of molecules and crystals. The main features of density functional theory are described and DFT…

Chemical Physics · Physics 2012-06-12 Hauke Paulsen , Alfred Xaver Trautwein

A challenge in modeling time-dependent strong-field processes such as high-harmonic generation for many-body systems, is how to effectively represent the electronic continuum. We apply Rothe's method to the time-dependent Hartree-Fock…

Chemical Physics · Physics 2025-08-22 Simon Elias Schrader , Håkon Emil Kristiansen , Thomas Bondo Pedersen , Simen Kvaal

We present a simple and efficient method to incorporate anharmonic effects in the vibrational \textcolor{black}{analyses} of molecules within density functional theory (DFT) calculations. This approach is closely related to the traditional…

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