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Related papers: Simulating X-ray absorption spectra with CASSCF li…

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We present a new approach for simulating X-ray absorption spectra based on linear-response density cumulant theory (LR-DCT) [A. V. Copan and A. Yu. Sokolov, J. Chem. Theory Comput., 2018, 14, 4097 - 4108]. Our new method combines the…

Chemical Physics · Physics 2019-06-03 Ruojing Peng , Andreas V. Copan , Alexander Yu. Sokolov

We explore Davidson methods for obtaining excitation energies and other linear response properties within quantum self-consistent linear response (q-sc-LR) theory. Davidson-type methods allow for obtaining only a few selected excitation…

We present an efficient implementation of the second-order two-component relativistic core-valence-separated algebraic diagrammatic construction method (CVS-ADC(2)) for core-excitation calculations. The approach employs state-averaged…

Chemical Physics · Physics 2026-05-01 Somesh Chamoli , Sudipta Chakraborty , Xubo Wang , Achintya Kumar Dutta

L-edge X-ray absorption spectra for first-row transition metal complexes are obtained from relativistic equation-of-motion singles and doubles coupled-cluster (EOM-CCSD) calculations that make use of the core-valence separation (CVS)…

X-ray absorption spectroscopy is a crucial experimental technique for elucidating the mechanisms of structural degradation in battery materials. However, extracting information from the measured spectrum is challenging without high-quality…

X-ray absorption spectroscopy (XAS) is a leading technique for understanding structural changes in advanced battery materials such as lithium-excess cathodes. However, extracting critical information like oxidation states from the…

X-ray interaction with matter is an energy-dependent process that is contingent on the atomic structure of the constituent material elements. The most advanced models to capture this relationship currently rely on Monte Carlo (MC)…

Machine Learning · Computer Science 2023-07-11 Raziye Kubra Kumrular , Thomas Blumensath

Widely employed Near-Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy probes a system by excitation of core electrons to unoccupied states. A variety of different methodologies are available to simulate corresponding spectra from…

Chemical Physics · Physics 2019-02-14 Georg S. Michelitsch , Karsten Reuter

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

We present the theory and implementation of a core-valence separated similarity transformed EOM-CCSD (STEOM-CCSD) method for K-edge core excitation spectra. The method can select an appropriate active space using CIS natural orbitals and…

Chemical Physics · Physics 2020-11-03 Santosh Ranga , Achintya Kumar Dutta

For the calculation of core-excited states probed through X-ray absorption spectroscopy, the core-valence separation (CVS) scheme has become a vital tool. This approach allows to target such states with high specificity, albeit introducing…

Chemical Physics · Physics 2020-08-26 Michael F. Herbst , Thomas Fransson

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 report a new theoretical method for X-ray absorption spectroscopy (XAS) in condensed matter which is based on the multi-channel multiple scattering theory of Natoli et al. and the eigen-channel R-matrix method. While the highly flexible…

Materials Science · Physics 2009-11-10 Peter Krüger , Calogero R. Natoli

First principle theoretical modeling of out-of-equilibrium processes observed in attosecond pump-probe transient absorption spectroscopy (TAS) triggering pure electron dynamics remains a challenging task, specially for heavy elements and/or…

Chemical Physics · Physics 2023-02-14 Torsha Moitra , Lukas Konecny , Marius Kadek , Angel Rubio , Michal Repisky

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

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

We present an algorithm to solve the CASSCF linear response equations that is both simple and efficient. The algorithm makes use of the well established symmetric and antisymmetric combinations of trial vectors, but further orthogonalizes…

Chemical Physics · Physics 2023-07-27 Riccardo Alessandro , Ivan Giannì , Federica Pes , Tommaso Nottoli , Filippo Lipparini

We present a scalable implementation of the $GW$ approximation using Gaussian atomic orbitals to study the valence and core ionization spectroscopies of molecules. The implementation of the standard spectral decomposition approach to the…

Chemical Physics · Physics 2021-12-06 Daniel Mejia-Rodriguez , Alexander Kunitsa , Edoardo Aprà , Niranjan Govind

Analytic energy gradients are presented for a variational two-electron reduced-density-matrix-driven complete active space self-consistent field (v2RDM-CASSCF) procedure that employs the density-fitting (DF) approximation to the…

Chemical Physics · Physics 2018-11-29 J. Wayne Mullinax , Evgeny Epifanovsky , Gergely Gidofalvi , A. Eugene DePrince

Spectroscopy is an indispensable tool in understanding the structures and dynamics of molecular systems. However computational modelling of spectroscopy is challenging due to the exponential scaling of computational complexity with system…

Quantum Physics · Physics 2021-06-22 Chee-Kong Lee , Chang-Yu Hsieh , Shengyu Zhang , Liang Shi
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