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Electrodynamical coupled cluster (CC) methodologies have been formulated employing standard QED Hamiltonian that is written in Coulomb gauge while using the DF and the MCDF pictures of the matter field for closed-shell and open-shell cases…

量子物理 · 物理学 2024-01-15 Sambhu N. Datta

Unitary coupled cluster (UCC), originally developed as a variational alternative to the popular traditional coupled cluster method, has seen a resurgence as a functional form for use on quantum computers. However, the number of excitors…

化学物理 · 物理学 2021-01-07 Maria-Andreea Filip , Alex J. W. Thom

In this work, we extend the dual triply irreducible local expansion (D-TRILEX) approach for correlated electronic systems by introducing a cluster reference system for the diagrammatic expansion. This framework allows us to consistently…

强关联电子 · 物理学 2026-02-26 Félix Fossati , Evgeny A. Stepanov

We report the implementation of a cost-effective approximation method within the framework of time-dependent optimized coupled-cluster (TD-OCC) method [J. Chem. Phys. 148, 051101 (2018)] for real-time simulations of intense laser-driven…

化学物理 · 物理学 2020-04-22 Himadri Pathak , Takeshi Sato , Kenichi L. Ishikawa

Introducing an active space approximation is inevitable for the quantum computations of chemical systems. However, this approximation ignores the electron correlations related to non-active orbitals. Here, we propose a computational method…

量子物理 · 物理学 2024-06-06 Luca Erhart , Yuichiro Yoshida , Viktor Khinevich , Wataru Mizukami

A novel implementation of the coupled-cluster singles and doubles (CCSD) approach is presented that is specifically tailored for the treatment of large, symmetric systems. It fully exploits Abelian point-group symmetry and the use of the…

化学物理 · 物理学 2023-12-07 Tommaso Nottoli , Jürgen Gauss , Filippo Lipparini

State-specific orbital optimized approaches are more accurate at predicting core-level spectra than traditional linear-response protocols, but their utility had been restricted on account of the risk of `variational collapse' down to the…

Density functional theory (DFT) provides convenient electronic structure methods for the study of molecular systems and materials. Regular Kohn-Sham DFT calculations rely on unitary transformations to determine the ground-state electronic…

化学物理 · 物理学 2022-10-10 Greta Jacobson , Juan M. Marmolejo-Tejada , Martín A. Mosquera

Exploiting Chemical Short-Range Order (CSRO) is a promising avenue for manipulating the properties of alloys. However, existing modeling frameworks are not sufficient to predict CSRO in multicomponent alloys (>3 components) in an efficient…

材料科学 · 物理学 2024-02-16 Chu-Liang Fu , Rajendra Prasad Gorrey , Bi-Cheng Zhou

One of the most important open challenges in modern Kohn-Sham (KS) density-functional theory (DFT) is the correct treatment of fractional electron charges and spins. Approximate exchange-correlation (XC) functionals struggle to do this in a…

化学物理 · 物理学 2015-12-24 Jonathan Nafziger , Adam Wasserman

Due to efficient scaling with electron number N, density functional theory (DFT) is widely used for studies of large molecules and solids. Restriction of an exact mean-field theory to local potential functions has recently been questioned.…

其他凝聚态物理 · 物理学 2015-06-24 Robert K. Nesbet

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…

材料科学 · 物理学 2024-03-19 Hyeondeok Shin , Kevin Gasperich , Tomas Rojas , Anh T. Ngo , Jaron T. Krogel , Anouar Benali

We consider a new formulation of the stochastic coupled cluster method in terms of the similarity transformed Hamiltonian. We show that improvement in the granularity with which the wavefunction is represented results in a reduction in the…

化学物理 · 物理学 2016-02-02 Ruth S. T. Franklin , James S. Spencer , Alberto Zoccante , Alex J. W. Thom

Long-range electrostatics and polarization remain central obstacles to extending machine learning interatomic potentials (MLIPs) to ionic, polar, and interfacial systems. Here, we introduce a semi-local framework for learning electrostatics…

In light of the recent discrepancies reported between fixed node diffusion Monte Carlo and local natural orbital coupled cluster with single, double and perturbative triples (CCSD(T)) methodologies for non-covalent interactions in large…

化学物理 · 物理学 2024-11-22 S. Lambie , D. Kats , D. Usyvat , A. Alavi

We implement a multi-orbital cluster dynamical mean-field theory (DMFT), by improving a sample-update algorithm in the continuous-time quantum Monte Carlo method based on the interaction expansion. The proposed sampling scheme for the…

强关联电子 · 物理学 2014-08-20 Yusuke Nomura , Shiro Sakai , Ryotaro Arita

The nucleation kinetics of the rotator phase in hard cuboctahedra, truncated octahedra, and rhombic dodecahedra is simulated via a combination of Forward Flux Sampling and Umbrella Sampling. For comparable degree of supersaturation, the…

软凝聚态物质 · 物理学 2015-06-17 Vikram Thapar , Fernando A. Escobedo

Lossy compression is widely used to reduce storage and I/O costs for large-scale particle datasets in scientific applications such as cosmology, molecular dynamics, and fluid dynamics, where clustering structures (e.g., single-linkage or…

机器学习 · 计算机科学 2026-04-22 Congrong Ren , Sheng Di , Katrin Heitmann , Franck Cappello , Hanqi Guo

Multi-configurational wave functions are known to describe electronic structure across a Born-Oppenheimer surface qualitatively correct. However, for quantitative reaction energies, dynamical correlation originating from the many…

化学物理 · 物理学 2020-04-16 Christopher J. Stein , Markus Reiher

We investigate the use of orbital-optimized references in conjunction with single-reference coupled-cluster theory with single and double substitutions (CCSD) for the study of core excitations and ionizations of 18 small organic molecules,…