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Valence excitation spectra are computed for all deep-center silicon-vacancy defect types in 3C, 4H, and 6H silicon carbide (SiC) and comparisons are made with literature photoluminescence measurements. Nuclear geometries surrounding the…

Chemical Physics · Physics 2018-03-14 Jesse J. Lutz , Xiaofeng F. Duan , Larry W. Burggraf

The chaotic nature of x-ray free-electron-laser pulses is a major bottleneck that has limited the joint temporal and spectral resolution of spectroscopic measurements. We show how to use the stochastic x-ray field statistics to overcome…

Optics · Physics 2021-02-15 Stefano M. Cavaletto , Daniel Keefer , Shaul Mukamel

A new perturbative approach to canonical equation-of-motion coupled-cluster theory is presented using coupled-cluster perturbation theory. A second-order M{\o}ller-Plesset partitioning of the Hamiltonian is used to obtain the well known…

Chemical Physics · Physics 2015-07-09 Jason N. Byrd , Varun Rishi , Ajith Perera , Rodney J. Bartlett

In this study, we demonstrate coherent optical excitation of the electronic Raman transition between the $1s\left(A_1\right)$ and $1s\left(E\right)$ split states of phosphorus donor in crystalline silicon. The dynamics of the generated…

Mesoscale and Nanoscale Physics · Physics 2026-02-05 Adam Gindl , Martin Čmel , František Trojánek , Petr Malý , Zbyněk Šobáň , Alexandr Pošta , Martin Kozák

The global optimum for valence population transfer in the NO$_2$ molecule driven by impulsive x-ray stimulated Raman scattering of one-femtosecond x-ray pulses tuned below the Oxygen K-edge is determined with the Multiconfiguration…

Computational Physics · Physics 2017-10-05 Daniel J. Haxton

This is the first attempt to construct detailed X-ray spectra of clusters of galaxies from the results of high-resolution hydrodynamic simulations and simulate X-ray observations in order to study velocity fields of the intracluster medium…

Astrophysics · Physics 2009-11-10 Yutaka Fujita , Tomoaki Matsumoto , Keiichi Wada , Tae Furusho

The accurate calculation of excited state properties of interacting electrons in the condensed phase is an immense challenge in computational physics. Here, we use state-of-the-art equation-of-motion coupled-cluster theory with single and…

Chemical Physics · Physics 2019-07-10 Alan M. Lewis , Timothy C. Berkelbach

We investigate the wavelength dependent ionization, heating, and expansion dynamics of medium-sized rare-gas clusters (Ar$_{923}$) under intense femtosecond short-wavelength free electron laser pulses by quasi-classical molecular dynamics…

Atomic and Molecular Clusters · Physics 2015-05-20 Mathias Arbeiter , Thomas Fennel

We present an implementation of equation of motion coupled-cluster singles and doubles (EOM-CCSD) theory using periodic boundary conditions and a plane wave basis set. Our implementation of EOM-CCSD theory is applied to study $F$-centers in…

Materials Science · Physics 2021-02-09 Alejandro Gallo , Felix Hummel , Andreas Irmler , Andreas Grüneis

We present an ab initio study of electronically excited states of three-dimensional solids using Gaussian-based periodic equation-of-motion coupled-cluster theory with single and double excitations (EOM-CCSD). The explicit use of…

Materials Science · Physics 2020-01-31 Xiao Wang , Timothy C. Berkelbach

A vibrational wavepacket in SF$_6$, created by impulsive stimulated Raman scattering with a few-cycle infrared pulse, is mapped onto five sulfur core-excited states using table-top soft X-ray transient absorption spectroscopy between…

We report an ultrafast and efficient way to create the maximum coherence between the two lower states in a -like atomic systems, driven by two nonlinearly chirped few-cycle pulses. The phenomenon of coherent population trapping and…

Quantum Physics · Physics 2011-11-18 Amarendra K. Sarma , Parvendra Kumar

A simple scheme of population and detection of low-lying electronic quadrupole modes in free small deformed metal clusters is proposed. The scheme is analyzed in terms of the TDLDA (time-dependent local density approximation) calculations.…

Atomic and Molecular Clusters · Physics 2014-02-04 V. O. Nesterenko , P. -G. Reinhard , T. Halfmann , L. I. Pavlov

In the molecular quantum chemistry community, coupled-cluster (CC) methods are well-recognized for their systematic convergence and reliability. The extension of the theory to extended systems has been comparably recent, so that…

Chemical Physics · Physics 2024-10-31 Andreas Grüneis , Evgeny Moerman , Matthias Scheffler , Tonghao Shen , Igor Ying Zhang

Quantum embedding methods have recently developed significantly to model large molecular structures. This work proposes a novel wave function theory in density functional theory (WTF-in-DFT) embedding scheme based on pair-coupled cluster…

Chemical Physics · Physics 2024-01-10 Rahul Chakraborty , Katharina Boguslawski , Paweł Tecmer

In single-reference coupled-cluster (CC) methods, one has to solve a set of non-linear polynomial equations in order to determine the so-called amplitudes which are then used to compute the energy and other properties. Although it is of…

Chemical Physics · Physics 2021-09-10 Antoine Marie , Fábris Kossoski , Pierre-François Loos

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

In this paper, we analyze the properties of the recently proposed real-time equation-of-motion coupled-cluster (RT-EOM-CC) cumulant Green's function approach [J. Chem. Phys. 2020, 152, 174113]. We specifically focus on identifying the…

Chemical Physics · Physics 2024-10-07 Bo Peng , Himadri Pathak , Ajay Panyala , Fernando D. Vila , John J. Rehr , Karol Kowalski

We demonstrate theoretically and numerically that laser-driven many-electron dynamics, as described by bivariational time-dependent coupled-cluster theory, may be analyzed in terms of stationary-state populations. Projectors heuristically…

Excited-state vibrations are crucial for determining photophysical and photochemical properties of molecular compounds. Stimulated Raman scattering can coherently stimulate and probe molecular vibrations with optical pulses, but it is…

Optics · Physics 2020-10-13 Giovanni Batignani , Carino Ferrante , Tullio Scopigno