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Simulations of laser-induced electron dynamics in a molecular system are performed using time-dependent (TD) equation-of-motion (EOM) coupled-cluster (CC) theory. The target system has been chosen to highlight potential shortcomings of…

Chemical Physics · Physics 2023-08-09 Stephen H. Yuwono , Brandon C. Cooper , Tianyuan Zhang , Xiaosong Li , A. Eugene DePrince

Time-dependent quantum chemical methods coupled to Gaussian basis sets are gaining popularity in modeling the electron dynamics of atoms and molecules interacting with intense laser fields. Two approaches most widely used for this purpose,…

Chemical Physics · Physics 2023-01-18 Aleksander P. Woźniak , Maciej Lewenstein , Robert Moszyński

We present the numerical implementation of the time-dependent complete-active-space self-consistent-field (TD-CASSCF) method [Phys. Rev. A, 88, 023402 (2013)] for atoms driven by a strong linearly polarized laser pulse. The present…

We develop a time-dependent multi-configurational numerical technique for calculating ionization by short laser pulses of many-electron molecules. The method is based on the expansion of the wave function of a molecule into the eigenstates…

Atomic Physics · Physics 2024-05-22 Vladislav V. Serov

While providing a highly accurate framework for simulating laser-induced many-electron dynamics in atom and molecules, including linear and nonlinear steady-state and transient absorption spectra, time-dependent coupled-cluster theory does…

The time-dependent equation-of-motion coupled cluster (TD-EOM-CC) and time-dependent coupled cluster (TDCC) methods are compared by simulating Rabi oscillations for different numbers of non-interacting atoms in a classical electromagnetic…

Chemical Physics · Physics 2023-10-02 Andreas S. Skeidsvoll , Henrik Koch

We present a wave-function based method to solve the time-dependent many-electron Schr\"odinger equation (TDSE) with special emphasis on strong-field ionization phenomena. The theory builds on the configuration-interaction (CI) approach…

Quantum Physics · Physics 2014-12-11 Sebastian Bauch , Lasse Kragh Sørensen , Lars Bojer Madsen

We formulate a time-dependent Fluctuating Local Field (TD-FLF) method for correlated fermion dynamics, extending the stationary FLF approach. The wavefunction is approximated as an ensemble of non-interacting states subject to a classical…

Strongly Correlated Electrons · Physics 2026-04-30 L. D. Silakov , Ya. S. Lyakhova , A. N. Rubtsov

Multi-configuration range-separated density-functional theory is extended to the time-dependent regime. An exact variational formulation is derived. The approximation, which consists in combining a long-range…

Chemical Physics · Physics 2013-02-27 Emmanuel Fromager , Stefan Knecht , Hans Jørgen Aa. Jensen

If one-electron observables of a many-electron system are of interest, a many-electron dynamics can be represented exactly by a one-electron dynamics with effective potentials. The formalism for this reduction is provided by the Exact…

Chemical Physics · Physics 2021-01-04 Jakub Kocák , Axel Schild

A time-dependent equation of motion coupled cluster singles and doubles (TD-EOM-CCSD) method is implemented, which uses a reduced basis calculated with the asymmetric band Lanczos algorithm. The approach is used to study weak-field…

It has been known that the time-dependent Hartree-Fock (TDHF) method, or the time-dependent density functional theory (TDDFT), fails to describe many-body quantum tunneling. We overcome this problem by superposing a few time-dependent…

Nuclear Theory · Physics 2020-06-15 N. Hasegawa , K. Hagino , Y. Tanimura

By simulating the real-time multielectron wavefunction with the multi-configurational time-dependent Hartree-Fock (MCTDHF) approach, we conduct an \textit{ab initio} study of the single-photon ionization process of a body-fixed water…

Atomic Physics · Physics 2026-01-14 Zhao-Han Zhang , Yang Li , Himadri Pathak , Takeshi Sato , Kenichi L. Ishikawa , Feng He

In this contribution, we extend our framework for analyzing and visualizing correlated many-electron dynamics to non-variational, highly scalable electronic structure method. Specifically, an explicitly time-dependent electronic wave packet…

Chemical Physics · Physics 2017-04-27 Gunter Hermann , Vincent Pohl , Jean Christophe Tremblay

The multiconfiguration time-dependent Hartree-Fock (MCTDHF) method is formulated for treating the coupled electronic and nuclear dynamics of diatomic molecules without the Born- Oppenheimer approximation. The method treats the full…

Computational Physics · Physics 2015-05-27 Daniel J. Haxton , Keith V. Lawler , C. William McCurdy

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

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 structure of approximate two electron wavefunction is deeply investigated, both theoretically and numerically, in the strong-field driven ionization dynamics. Theoretical analyses clarify that for two electron singlet systems, the…

Atomic Physics · Physics 2014-11-13 Takeshi Sato , Kenichi L Ishikawa

We present a numerical implementation of the infinite-range exterior complex scaling (irECS) [Phys. Rev. A 81, 053845 (2010)] as an efficient absorbing boundary to the time-dependent complete-active-space self-consistent field (TD-CASSCF)…

Atomic Physics · Physics 2018-03-07 Yuki Orimo , Takeshi Sato , Armin Scrinzi , Kenichi L. Ishikawa

We show that quantum optimal control theory (OCT) and time-dependent density-functional theory (TDDFT) can be combined to provide realistic femtosecond laser pulses for an enhanced ionization yield in many-electron systems. Using the…

Atomic Physics · Physics 2015-06-17 M. Hellgren , E. Rasanen , E. K. U. Gross