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The success of the "Cluster Variation Method" (CVM) in reproducing quite accurately the free energies of Monte Carlo (MC) calculations on Ising models is explained in terms of identifying a cancellation of errors: We show that the CVM…

Materials Science · Physics 2009-10-31 Luiz G. Ferreira , C. Wolverton , Alex Zunger

We discuss diagrammatic modifications to the coupled cluster doubles (CCD) equations, wherein different groups of terms out of rings, ladders, crossed-rings and mosaics can be removed to form approximations to the coupled cluster method, of…

Chemical Physics · Physics 2014-05-06 James J. Shepherd , Thomas. M. Henderson , Gustavo E. Scuseria

Compared to common density functionals, ab initio wave function methods can provide greater reliability and accuracy, which could prove useful when modeling adsorbates or defects of otherwise periodic systems. However, the breaking of…

Materials Science · Physics 2020-10-02 Bryan T. G. Lau , Gerald Knizia , Timothy C. Berkelbach

First-principles calculations are a cornerstone of modern surface science and heterogeneous catalysis. However, accurate reaction energies and barrier heights are frequently inaccessible due to the approximations demanded by the large…

Materials Science · Physics 2024-02-08 Hong-Zhou Ye , Timothy C. Berkelbach

We develop a static quantum embedding scheme that utilizes different levels of approximations to coupled cluster (CC) theory for an active fragment region and its environment. To reduce the computational cost, we solve the local fragment…

Chemical Physics · Physics 2024-11-13 Avijit Shee , Fabian M. Faulstich , Birgitta Whaley , Lin Lin , Martin Head-Gordon

In this paper, we apply multi-task Gaussian Process (MT-GP) to show that the adsorption energy of small adsorbates on transition metal surfaces can be modeled to a high level of fidelity using data from multiple sources, taking advantage of…

Data Analysis, Statistics and Probability · Physics 2019-01-29 Huijie Tian , Srinivas Rangarajan

The simulation of the development of cascade processes in calorimeters of different types for the implementation of energy measurement by correlation curves method, is carried out. Heterogeneous calorimeter has a significant transient…

Instrumentation and Methods for Astrophysics · Physics 2014-11-04 E. A. Grushevskaya , I. A. Lebedev , A. I. Fedosimova

A relativistic version of the coupled-cluster single-double (CCSD) method is developed for atoms with a single valence electron. In earlier work, a linearized version of the CCSD method (with extensions to include a dominant class of triple…

Atomic Physics · Physics 2009-11-13 Rupsi Pal , M. S. Safronova , W. R. Johnson , Andrei Derevianko , Sergey G. Porsev

The recent quantum information boom has effected a resurgence of interest in unitary coupled cluster (UCC) theory. Our group's interest in local energy landscapes of unitary ans\"atze prompted us to investigate the classical approach of…

Chemical Physics · Physics 2022-11-01 Harper R. Grimsley , Nicholas J. Mayhall

The effect of an oscillating electric field normal to a metallic surface may be described by an effective potential. This induced potential is calculated using semiclassical variants of the random phase approximation (RPA). Results are…

Mesoscale and Nanoscale Physics · Physics 2016-08-31 Michael Wilkinson

Recent disagreement between state-of-the-art quantum chemical methods, coupled cluster with single, double and perturbative triples excitations and fixed-node diffusion Monte Carlo, calls for systematic examination of possible sources of…

Chemical Physics · Physics 2025-05-14 S. Lambie , C. Rickert , D. Usvyat , A. Alavi , D. Kats

A first-principles study of the adsorption of a single water molecule on a layer of graphitic carbon nitride employing an embedding approach is presented. The embedding approach involves an algorithm to obtain localized Wannier orbitals of…

Chemical Physics · Physics 2022-01-11 Tobias Schäfer , Alejandro Gallo , Andreas Irmler , Felix Hummel , Andreas Grüneis

We investigate the convergence of coupled-cluster correlation energies and related quantities with respect to the employed basis set size for the uniform electron gas to gain a better understanding of the basis set incompleteness error. To…

Materials Science · Physics 2024-02-27 Nikolaos Masios , Felix Hummel , Andreas Grüneis , Andreas Irmler

In the framework of the computational determination of highly-accurate vertical excitation energies in small organic compounds, we explore the possibilities offered by the equation-of-motion formalism relying on the approximate fourth-order…

We present an algorithm for accelerating the search of molecule's adsorption site based on global optimization of surface adsorbate geometries. Our approach uses a machine-learning interatomic potential (moment tensor potential) to…

Materials Science · Physics 2024-12-30 Olga Klimanova , Nikita Rybin , Alexander Shapeev

The photoabsorption spectra of calcium-doped argon clusters CaAr_n are investigated at thermal equilibrium using a variety of theoretical and numerical tools. The influence of temperature on the absorption spectra is estimated using the…

Chemical Physics · Physics 2009-11-07 F. Calvo , F. Spiegelman , M. C. Heitz

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…

Quantum Physics · Physics 2024-06-06 Luca Erhart , Yuichiro Yoshida , Viktor Khinevich , Wataru Mizukami

Some methods for the convergence acceleration of the M{\o}ller-Plesset perturbation series for the correlation energy are discussed. The order-by-order summation is less effective than the Feenberg series. The latter is obtained by…

chem-ph · Physics 2011-08-22 Herbert H. H. Homeier

We reveal limitations of several standard coupled-cluster (CC) methods with perturbation-theorybased noniterative or approximate iterative treatments of triple excitations when applied to thedetermination of highly accurate potential energy…

Chemical Physics · Physics 2021-10-04 Jan Schnabel , Lan Cheng , Andreas Köhn

In this work we propose a novel composite method for accurate calculation of the energies of many-electron atoms. The dominant contribution to the energy (pair energies) are calculated by using explicitly correlated factorisable coupled…

Atomic Physics · Physics 2018-12-12 Michal Przybytek , Michal Lesiuk
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