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A mixed quantum-classical approach to simulate the coupled dynamics of electrons and nuclei in nanoscale molecular systems is presented. The method relies on a second order expansion of the Lagrangian in time-dependent density functional…

Chemical Physics · Physics 2009-11-10 T. A. Niehaus , D. Heringer , B. Torralva , Th. Frauenheim

A major difficulty in quantum simulation is the adequate treatment of a large collection of entangled particles, synonymous with electron correlation in electronic structure theory, with coupled cluster (CC) theory being the leading…

Chemical Physics · Physics 2024-06-06 Zachary W. Windom , Daniel Claudino , Rodney J. Bartlett

The performance of time-independent, orbital optimized calculations of excited states is assessed with respect to charge transfer excitations in organic molecules in comparison to the linear-response time-dependent density functional theory…

Chemical Physics · Physics 2024-05-22 Elli Selenius , Alec Elías Sigurdarson , Yorick L. A. Schmerwitz , Gianluca Levi

One method of representing a high-rank tensor as a (hyper-)product of lower-rank tensors is the tensor hypercontraction (THC) method of Hohenstein et al. This strategy has been found to be useful for reducing the polynomial scaling of…

Chemical Physics · Physics 2025-03-26 Avdhoot Datar , Devin A. Matthews

The primary computational challenge when simulating nonadiabatic ab initio molecular dynamics is the unfavorable compute costs of electronic structure calculations with molecular size. Simple electronic structure theories, like…

Chemical Physics · Physics 2023-06-28 Justin J. Talbot , Martin Head-Gordon , Stephen J. Cotton

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

The extension of the highly-optimized local natural orbital (LNO) CCSD(T) method is presented for high-spin open-shell molecules. The techniques enabling the outstanding efficiency of the closed-shell LNO-CCSD(T) variant are adopted,…

Chemical Physics · Physics 2023-11-17 P. Bernát Szabó , József Csóka , Mihály Kállay , Péter R. Nagy

The previously proposed ansatz for density cumulant theory that combines orbital-optimization and a parameterization of the 2-electron reduced density matrix cumulant in terms of unitary coupled cluster amplitudes (OUDCT) is carefully…

Chemical Physics · Physics 2020-12-23 Jonathon P. Misiewicz , Justin M. Turney , Henry F. Schaefer , Alexander Yu. Sokolov

Electronic circular dichroism (ECD) is a powerful spectroscopical method for investigating chiral properties at the molecular level. ECD calculations with the commonly used linear-response time-dependent density functional theory (LR-TDDFT)…

We analytically study the Out-of-Time-Order Correlation functions (OTOC) for two spatially separated primary operators in two-dimensional unitary minimal models. Besides giving general arguments using the conformal symmetry, we also use the…

High Energy Physics - Theory · Physics 2018-09-20 Ruihua Fan

We have studied electron correlations in the doped two-dimensional (2D) Hubbard model by using the coupled-cluster method (CCM) to investigate whether or not the method can be applied to correct the independent particle approximations…

Strongly Correlated Electrons · Physics 2009-10-31 Yoshihiro Asai , Hideki Katagiri

Localized molecular orbitals are often used for the analysis of chemical bonds, but they can also serve to efficiently and comprehensibly compute linear response properties. While conventional canonical molecular orbitals provide an…

Chemical Physics · Physics 2023-02-08 Souloke Sen , Bruno Senjean , Lucas Visscher

The problem of orbital relaxation in computational core-hole spectroscopies, including x-ray absorption and x-ray photoionization, has long plagued linear response approaches, including equation-of-motion coupled cluster with singles and…

Chemical Physics · Physics 2025-03-26 Megan E. Simons , Devin A. Matthews

We propose a streamlined combination scheme of the transcorrelation (TC) and coupled cluster (CC) theory, which not only increases the convergence rate with respect to the basis set, but also extends the applicability of the lowest order CC…

Strongly Correlated Electrons · Physics 2021-07-28 Ke Liao , Thomas Schraivogel , Hongjun Luo , Daniel Kats , Ali Alavi

We introduce a new implementation of the coupled cluster method tailored by matrix product states wave functions (DMRG-TCCSD), which employs the local pair natural orbital approach (LPNO). By exploiting locality in the coupled cluster stage…

Chemical Physics · Physics 2020-01-16 Andrej Antalík , Libor Veis , Jiří Brabec , Örs Legeza , Jiří Pittner

We present a generalized formulation of the Optimized Effective Potential (OEP) approach to the Self Interaction Correction (SIC) problem in Time Dependent (TD) Density Functional Theory (DFT). The formulation relies on the introduction of…

Quantum Physics · Physics 2016-02-03 J. Messud , P. M. Dinh , P. -G. Reinhard , E. ~Suraud

Here we demonstrate workably accurate estimation of optical excitation threshold for large systems comprising of hundreds of atoms through an anti-causally corrected(ACC) real-time dynamics(RTD) approach implemented in a minimal…

Materials Science · Physics 2023-06-13 Joydev De , Manoar Hossain , Joydeep Bhattacharjee

The time-dependent density functional theory (TDDFT) has been broadly used to investigate the excited-state properties of various molecular systems. However, the current TDDFT heavily relies on outcomes from the corresponding ground-state…

Chemical Physics · Physics 2020-09-02 Shu-Hao Yeh , Aaditya Manjanath , Yuan-Chung Cheng , Jeng-Da Chai , Chao-Ping Hsu

We introduce a unitary coupled-cluster (UCC) ansatz termed $k$-UpCCGSD that is based on a family of sparse generalized doubles (D) operators which provides an affordable and systematically improvable unitary coupled-cluster wavefunction…

Quantum Physics · Physics 2019-01-07 Joonho Lee , William J. Huggins , Martin Head-Gordon , K. Birgitta Whaley

A time-dependent vibrational electronic coupled-cluster (VECC) approach is proposed to simulate photoelectron/ UV-VIS absorption spectra, as well as time-dependent properties for non-adiabatic vibronic models, going beyond the…

Chemical Physics · Physics 2023-12-25 Songhao Bao , Neil Raymond , Marcel Nooijen