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We investigate the coupling of different quantum-embedding approaches with a third molecular-mechanics layer, which can be either polarizable or non-polarizable. In particular, such a coupling is discussed for the multilevel families of…

Chemical Physics · Physics 2020-12-11 Linda Goletto , Tommaso Giovannini , Sarai D. Folkestad , Henrik Koch

We present a stable and systematically improvable quantum Monte Carlo (QMC) approach to calculating excited-state energies, which we implement using our fast randomized iteration method for the full configuration interaction problem…

Computational Physics · Physics 2023-10-03 Samuel M. Greene , Robert J. Webber , James E. T. Smith , Jonathan Weare , Timothy C. Berkelbach

We present a systematic study of the correlation-induced corrections to the electronic band structure of zinc-blende BN. Our investigation employs an ab initio wave-function-based local Hamiltonian formalism which offers a rigorous approach…

Strongly Correlated Electrons · Physics 2010-12-20 A. Stoyanova , L. Hozoi , P. Fulde , H. Stoll

Accurate determination of electronic properties of correlated oxides remains a significant challenge for computational theory. Traditional Hubbard-corrected density functional theory (DFT+U) frequently encounters limitations in precisely…

Materials Science · Physics 2024-03-19 Hyeondeok Shin , Kevin Gasperich , Tomas Rojas , Anh T. Ngo , Jaron T. Krogel , Anouar Benali

Multiconfiguration Hartree-Fock (MCHF) and multiconfiguration Dirac-Hartree-Fock (MCDHF) calculations are performed for the $2p^{5}~^{2}P^{o}$, $2p^4(^{3}P)3s~^{4}P$, $2p^4(^{3}P)3s~^{2}P$ and $2p^4(^{3}P)3p~^{4}S^o$ states of $^{19}$F~I to…

Atomic Physics · Physics 2018-04-12 Nouria Aourir , Messaoud Nemouchi , Michel Godefroid , Per Jönsson

A method is presented in which the ground-state subspace is projected out of a Hamiltonian representation. As a result of this projection, an effective Hamiltonian is constructed where its ground-state coincides with an excited-state of the…

Quantum Physics · Physics 2023-08-14 P. Jouzdani , S. Bringuier , M. Kostuk

Computationally efficient and accurate quantum mechanical approximations to solve the many-electron Schr\"odinger equation are at the heart of computational materials science. In that respect the coupled cluster hierarchy of methods plays a…

Materials Science · Physics 2022-01-11 Tina N. Mihm , Tobias Schäfer , Sai Kumar Ramadugu , Andreas Grüneis , James J. Shepherd

This paper presents a nonperturbative treatment of strong-coupling induced effects in atom-field systems which cannot be seen in traditional perturbative treatments invoking compromising assumptions such as the Born-Markov, rotating wave or…

Quantum Physics · Physics 2020-02-25 Jen-Tsung Hsiang , Bei-Lok Hu

We develop an iterative diagonalization scheme in solving a one-body self-consistent-field equation in the transcorrelated (TC) method using a plane-wave basis set. Non-Hermiticity in the TC method is well handled with a block-Davidson…

Materials Science · Physics 2016-03-15 Masayuki Ochi , Yoshiyuki Yamamoto , Ryotaro Arita , Shinji Tsuneyuki

We present an excited-state-specific coupled-cluster approach in which both the molecular orbitals and cluster amplitudes are optimized for an individual excited state. The theory is formulated via a pseudoprojection of the traditional…

Chemical Physics · Physics 2023-11-27 Harrison Tuckman , Eric Neuscamman

In the context of Frenkel exciton dynamics in aggregated molecules the polaron transformation technique facilitates a treatment where diagonal elements attributed to electronic excited-state populations are decoupled from fluctuations…

Chemical Physics · Physics 2021-08-30 Joachim Seibt , Oliver Kühn

An excitonic method proper to study conjugated oligomers and polymers is described and its applicability tested on the ground state and first excited states of trans-polyacetylene, taken as a model. From the Pariser-Parr-Pople Hamiltonian,…

Condensed Matter · Physics 2009-10-31 S. Pleutin , J. L. Fave

This work develops and illustrates a new method of calculating "chemically accurate" electronic wavefunctions (and energies) via a truncated full configuration interaction (CI) procedure which arguably circumvents the large matrix…

Chemical Physics · Physics 2022-12-21 Stephen J. Cotton

The character of an electronically excited state is one of the most important descriptors employed to discuss the photophysics and photochemistry of transition metal complexes. In transition metal complexes, the interaction between the…

Chemical Physics · Physics 2018-02-14 Sebastian Mai , Felix Plasser , Johann Dorn , Maria Fumanal , Chantal Daniel , Leticia González

We present two improvements to the tight-binding approximation of time-dependent density functional theory (TD-DFTB): Firstly, we add an exact Hartree-Fock exchange term, which is switched on at large distances, to the ground state…

Chemical Physics · Physics 2015-10-28 Alexander Humeniuk , Roland Mitric

An ab initio Wannier-function-based approach to electronic ground-state calculations for crystalline solids is outlined. In the framework of the linear combination of atomic orbitals method the infinite character of the solid is rigorously…

Condensed Matter · Physics 2009-10-31 Martin Albrecht , Alok Shukla , Michael Dolg , Peter Fulde , Hermann Stoll

A procedure to obtain single-electron wavefunctions within the tight-binding formalism is proposed. It is based on linear combinations of Slater-type orbitals whose screening coefficients are extracted from the optical matrix elements of…

Materials Science · Physics 2016-09-16 R. Benchamekh , F. Raouafi , J. Even , F. Ben Cheikh Larbi , P. Voisin , J. -M. Jancu

The perturbatively selected configuration interaction scheme (CIPSI) is particularly effective in constructing determinantal expansions for quantum Monte Carlo (QMC) simulations with Jastrow-Slater wave functions: fast and smooth…

Classical Physics · Physics 2021-03-02 Monika Dash , Saverio Moroni , Claudia Filippi , Anthony Scemama

To analyze quantum many-body Hamiltonians, recently, machine learning techniques have been shown to be quite useful and powerful. However, the applicability of such machine learning solvers is still limited. Here, we propose schemes that…

Strongly Correlated Electrons · Physics 2020-04-17 Yusuke Nomura

Vibrational motions in electronically excited states can be observed by either time and frequency resolved infrared absorption or by off resonant stimulated Raman techniques. Multipoint correlation function expressions are derived for both…

Quantum Physics · Physics 2017-09-13 Konstantin E. Dorfman , Benjamin P. Fingerhut , Shaul Mukamel