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The development of reliable ab initio methods for light-matter strong coupling is necessary for a deeper understanding of molecular polaritons. The recently developed strong coupling quantum electrodynamics Hartree-Fock model (SC-QED-HF)…

Chemical Physics · Physics 2025-02-21 Matteo Castagnola , Rosario R. Riso , Yassir El Moutaoukal , Enrico Ronca , Henrik Koch

We present an exact single-electron picture that describes the correlated electron dynamics in strong laser fields. Our approach is based on the factorization of the electronic wavefunction as a product of a marginal and a conditional…

Chemical Physics · Physics 2017-04-26 Axel Schild , E. K. U. Gross

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…

In this paper we motivate, formulate and analyze the Multi-Configuration Time-Dependent Hartree-Fock (MCTDHF) equations for molecular systems under Coulomb interaction. They consist in approximating the N-particle Schrodinger wavefunction…

Mathematical Physics · Physics 2015-05-13 C. Bardos , I. Catto , N. Mauser , S. Trabelsi

We develop an analytical model of correlated two-electron ionization in strong infrared laser fields. The model includes all relevant interactions between the electrons, the laser field, and the ionic core nonperturbatively. We focus on the…

Atomic Physics · Physics 2009-02-14 Denys I. Bondar , Wing-Ki Liu , Misha Yu. Ivanov

We review different computational methods for the calculation of photoelectron spectra and angular distributions of atoms and molecules when excited by laser pulses using time-dependent density-functional theory (TDDFT) that are suitable…

Chemical Physics · Physics 2017-03-28 Philipp Wopperer , Umberto De Giovannini , Angel Rubio

The accurate description of the non-linear response of many-electron systems to strong-laser fields remains a major challenge. Methods that bypass the unfavorable exponential scaling with particle number are required to address larger…

We develop a time-dependent theory to investigate electron dynamics and photoionization processes of diatomic molecules interacting with strong laser fields including electron-electron correlation effects. We combine the recently formulated…

Chemical Physics · Physics 2016-02-02 Henrik R. Larsson , Sebastian Bauch , Lasse Kragh Sørensen , Michael Bonitz

We propose a framework to learn the time-dependent Hartree-Fock (TDHF) inter-electronic potential of a molecule from its electron density dynamics. Though the entire TDHF Hamiltonian, including the inter-electronic potential, can be…

Chemical Physics · Physics 2024-12-05 Harish S. Bhat , Prachi Gupta , Christine M. Isborn

This article examines the time-dependent Hartree-Fock (TDHF) approximation of single-particle dynamics in systems of interacting fermions. We find the TDHF approximation to be accurate when there are sufficiently many particles and the…

Mathematical Physics · Physics 2007-05-23 Claude Bardos , Francois Golse , Alex D. Gottlieb , Norbert J. Mauser

Modeling chemical reactions with quantum chemical methods is challenging when the electronic structure varies significantly throughout the reaction, as well as when electronic excited states are involved. Multireference methods such as…

Many-electron systems at substantial finite temperatures and densities present a major challenge to density functional theory. Very little is known about the free-energy behavior over the temperature range of interest, for example, in the…

Materials Science · Physics 2012-01-25 Travis Sjostrom , Frank E. Harris , S. B. Trickey

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

Time-dependent Hartree-Fock (TDHF) theory has been a powerful tool in describing a variety of complex nuclear dynamics microscopically without empirical parameters. In this contribution, recent advances in nuclear dynamics studies with TDHF…

Nuclear Theory · Physics 2019-03-26 Kazuyuki Sekizawa

Bichromatic extreme-ultraviolet pulses from a seeded free-electron laser enable us to measure photoelectron angular distribution (PAD) as a function of the relative phase between the different wavelength components. The time-dependent…

Atomic Physics · Physics 2021-05-26 Yuki Orimo , Oyunbileg Tugs , Takeshi Sato , Daehyun You , Kiyoshi Ueda , Kenichi L. Ishikawa

Density matrix embedding theory (DMET) is a fully quantum-mechanical embedding method which shows great promise as a method of defeating the inherent exponential cost scaling of multiconfigurational wave function-based calculations by…

Chemical Physics · Physics 2019-02-07 Matthew R. Hermes , Laura Gagliardi

We investigate the one-body dissipation dynamics in heavy-ion collisions of $^{16}{\rm O}$+$^{16}{\rm O}$ using a fully three-dimensional time-dependent Hartree-Fock (TDHF) theory with the modern Skyrme energy functional and without any…

Nuclear Theory · Physics 2015-06-23 Gao-Feng Dai , Lu Guo , En-Guang Zhao , Shan-Gui Zhou

We have verified a mechanism for Raman excitation of atoms through continuum levels previously obtained by quantum optimal control using the multi-configurational time-dependent Hartree-Fock (MCTDHF) method. For the optimal control, which…

Atomic Physics · Physics 2017-07-19 Loren Greenman , K. Birgitta Whaley , Daniel J. Haxton , C. William McCurdy

The present work explores quantitative limits to the Single-Active Electron (SAE) approximation, often used to deal with strong-field ionization and subsequent attosecond dynamics. Using a time-dependent multi\-configuration approach,…

Atomic Physics · Physics 2025-11-04 Jean-Nicolas Vigneau , Tung Nguyen-Dang , Eric Charron , Osman Atabek

This chapter provides a basic introduction to excited-state extensions of density functional theory (DFT), including time-dependent (TD-)DFT in both its linear-response and its explicitly time-dependent formulations. As applied to the…

Chemical Physics · Physics 2023-05-02 John M. Herbert