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The time-dependent complete-active-space self-consistent-field (TD-CASSCF) method for the description of multielectron dynamics in intense laser fields is presented, and a comprehensive description of the method is given. It introduces the…

Atomic Physics · Physics 2015-06-15 Takeshi Sato , Kenichi L. Ishikawa

We present a polarizable embedding quantum mechanics/molecular mechanics (QM/MM) framework for ground- and excited-state Complete Active Space Self-Consistent Field (CASSCF) calculations on molecules within complex environments, such as…

Chemical Physics · Physics 2024-11-20 Tommaso Nottoli , Mattia Bondanza , Filippo Lipparini , Benedetta Mennucci

Multicomponent methods seek to treat select nuclei, typically protons, fully quantum mechanically and equivalent to the electrons of a chemical system. In such methods, it is well known that due to the neglect of electron-proton…

Chemical Physics · Physics 2020-12-21 O. Jonathan Fajen , Kurt R. Brorsen

We present the time-dependent complete-active-space self-consistent-field (TD-CASSCF) method to simulate multielectron dynamics in ultrafast intense laser fields from the first principles. While based on multiconfiguration expansion, it…

Atomic Physics · Physics 2018-04-24 Takeshi Sato , Yuki Orimo , Takuma Teramura , Oyunbileg Tugs , Kenichi L. Ishikawa

The complete active space self-consistent field (CASSCF) method is the principal approach employed for studying strongly correlated systems. However, exact CASSCF can only be performed on small active spaces of ~20 electrons in ~20 orbitals…

Computational Physics · Physics 2021-12-22 Daniel S. Levine , Diptarka Hait , Norm M. Tubman , Susi Lehtola , K. Birgitta Whaley , Martin Head-Gordon

A multiscale model based on the coupling of the multiconfigurational self-consistent field (MCSCF) method and the classical atomistic polarizable Fluctuating Charges (FQ) force field is presented. The resulting MCSCF/FQ approach is…

We present a novel implementation of the complete active space self-consistent field (CASSCF) method that makes use of the many-body expanded full configuration interaction (MBE-FCI) method to incrementally approximate electronic structures…

Hybrid light-matter polaritonic states have shown great promise for altering already known and enabling novel chemical reactions and controlling photophysical phenomena. This field has recently become one of the most prominent and active…

Quantum Physics · Physics 2025-05-23 Braden M. Weight , Yu Zhang

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…

In this work, we investigate the possibility of improving multireference-driven coupled cluster (CC) approaches with an algorithm that iteratively combines complete active space (CAS) calculations with tailored CC and externally corrected…

Chemical Physics · Physics 2025-03-06 Robin Feldmann , Max Mörchen , Jakub Lang , Michał Lesiuk , Markus Reiher

The accurate resolution of the chemical properties of strongly correlated systems, such as biradicals, requires the use of electronic structure theories that account for both multi-reference as well as dynamic correlation effects. A variety…

Chemical Physics · Physics 2023-01-03 Jan-Niklas Boyn , David A. Mazziotti

New density functional theory approach based on a complete active space self-consistent field (CASSCF) reference function in Extended Koopmans' approximation is discussed. Recently, the number of generalizations of density functional theory…

Chemical Physics · Physics 2018-02-15 Sergey Gusarov , Yurii Dmitriev

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…

We present the time-dependent restricted-active-space self-consistent field (TD-RASSCF) theory as a new framework for the time-dependent many-electron problem. The theory generalizes the multiconfigurational time-dependent Hartree-Fock…

Atomic Physics · Physics 2014-05-22 Haruhide Miyagi , Lars Bojer Madsen

Polaritonic chemistry relies on the strong light-matter interaction phenomena for altering the chemical reaction rates inside optical cavities. To explain and to understand these processes, the development of reliable theoretical models is…

Chemical Physics · Physics 2022-09-14 Fabijan Pavošević , Angel Rubio

Multireference electron correlation methods describe static and dynamical electron correlation in a balanced way, and therefore, can yield accurate and predictive results even when single-reference methods or multiconfigurational…

Chemical Physics · Physics 2019-11-19 Jae Woo Park , Rachael Al-Saadon , Matthew K. MacLeod , Toru Shiozaki , Bess Vlaisavljevich

Computation of electronic spectra is one of the most important applications of methods capturing static electron correlation, including complete-active-space self-consistent field (CASSCF) and post-CASSCF theories. Performance of these…

Chemical Physics · Physics 2025-11-19 Reza G. Shirazi , Alexander Zech , Peter Pinski , Vladimir V. Rybkin

State-specific complete active space self-consistent field (SS-CASSCF) theory has emerged as a promising route to accurately predict electronically excited energy surfaces away from molecular equilibria. However, its accuracy and…

Chemical Physics · Physics 2024-02-21 Sandra Saade , Hugh G. A. Burton

The computation of excited states within the Complete Active Space Self-Consistent Field (CASSCF) framework remains a significant challenge in quantum chemistry, both theoretically and algorithmically. In this work, we extend the K\"ahler…

Chemical Physics · Physics 2026-04-16 Laura Grazioli , Yukuan Hu , Tommaso Nottoli , Filippo Lipparini , Eric Cancès

A comprehensive theoretical understanding of electron-photon correlation is essential for describing the reshaping of molecular orbitals in quantum electrodynamics (QED) environments. The strong coupling QED Hartree-Fock (SC-QED-HF) theory…

Chemical Physics · Physics 2024-09-04 Yassir El Moutaoukal , Rosario R. Riso , Matteo Castagnola , Henrik Koch
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