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The S66 non-covalent interactions are studied through localized coupled-cluster methods and general LNO-CCSD(T)-based composite schemes. Very small RMS deviations (\leq 0.05 kcal/mol) for the low-cost composite approaches from the SILVER…

Chemical Physics · Physics 2022-11-28 Emmanouil Semidalas , Golokesh Santra , Nisha Mehta , Jan M. L. Martin

Accurate solution of the many-electron problem including correlations remains intractable except for few-electron systems. Describing interacting electrons as a superposition of independent electron configurations results in an apparent…

Computational Physics · Physics 2024-02-20 J. C. Greer

In the present letter, it is demonstrated how full configuration interaction (FCI) results in extended basis sets may be obtained to within sub-kJ/mol accuracy by decomposing the energy in terms of many-body expansions in the virtual…

Chemical Physics · Physics 2017-09-15 Janus J. Eriksen , Filippo Lipparini , Jürgen Gauss

The BCS equations are the centerpiece of the microscopic description of superconductivity. Their space discretization yields a system of coupled ordinary differential equations. In this work, we come up with fast time evolution schemes…

Superconductivity · Physics 2015-10-19 Jonathan Seyrich

We describe a method for computing near-exact energies for correlated systems with large Hilbert spaces. The method efficiently identifies the most important basis states (Slater determinants) and performs a variational calculation in the…

Chemical Physics · Physics 2020-01-22 Junhao Li , Yuan Yao , Adam A. Holmes , Matthew Otten , Qiming Sun , Sandeep Sharma , C. J. Umrigar

Numerous numerical studies have shown that geminal-based methods are a promising direction to model strongly correlated systems with low computational costs. Several strategies have been introduced to capture the missing dynamical…

Chemical Physics · Physics 2023-03-22 Artur Nowak , Katharina Boguslawski

An adaptation of the full configuration interaction quantum Monte Carlo (FCIQMC) method is presented, for correlated electron problems containing heavy elements and the presence of significant relativistic effects. The modified algorithm…

Chemical Physics · Physics 2020-10-26 Robert J. Anderson , George H. Booth

Systems with long-range interactions have seen a surge of interest in the past decades. In the wake of this surge, the use of a system size dependent rescaling, sometimes termed "Kac prescription," of the long-range pair potential has seen…

Statistical Mechanics · Physics 2025-06-30 Michael Kastner

The stochastic resolution of identity (sRI) approximation significantly reduces the computational scaling of CC2 from O(N^5) to O(N^3), where N is a measure of system size. However, the inherent stochastic noise, while controllable, can…

Chemical Physics · Physics 2025-10-01 Chongxiao Zhao , Wenjie Dou

This paper gives performance limits of the segmented compressive sampling (CS) which collects correlated samples. It is shown that the effect of correlation among samples for the segmented CS can be characterized by a penalty term in the…

Information Theory · Computer Science 2016-03-03 Hao Fang , Sergiy A. Vorobyov , Hai Jiang

We extend the recently proposed heat-bath configuration interaction (HCI) method [Holmes, Tubman, Umrigar, J. Chem. Theory Comput. 12, 3674 (2016)], by introducing a semistochastic algorithm for performing multireference Epstein-Nesbet…

Chemical Physics · Physics 2017-03-20 Sandeep Sharma , Adam Holmes , Guillaume Jeanmairet , Ali Alavi , C. J. Umrigar

Exascale computing promises quantities of data too large to efficiently store and transfer across networks in order to be able to analyze and visualize the results. We investigate Compressive Sensing (CS) as a way to reduce the size of the…

Information Theory · Computer Science 2015-08-27 Maher Salloum , Nathan Fabian , David M. Hensinger , Jeremy A. Templeton

Machine learning interatomic potentials are revolutionizing large-scale, accurate atomistic modelling in material science and chemistry. Many potentials use atomic cluster expansion or equivariant message passing frameworks. Such frameworks…

Computational Physics · Physics 2024-07-31 Bingqing Cheng

In this paper, we develop a class of antisymmetrized geminal power configuration interaction (AGP-CI) wave functions that extend the AGP framework by incorporating inter-geminal correlations through a CI expansion. To make these…

Chemical Physics · Physics 2026-04-16 Airi Kawasaki , Fei Gao , Gustavo E. Scuseria

The aim of this paper is to investigate the links between ${\cal T}_C$-class algorithms, CQ Algorithm and shrinking projection methods. We show that strong convergence of these algorithms are related to coherent ${\cal T}_C$-class sequences…

Optimization and Control · Mathematics 2009-09-21 Jean-Philippe Chancelier

Background: Ab initio many-body methods have been developed over the past ten years to address mid-mass nuclei... As progress in the design of inter-nucleon interactions is made, further efforts must be made to tailor many-body methods.…

Nuclear Theory · Physics 2017-02-01 J. Ripoche , D. Lacroix , D. Gambacurta , J. -P. Ebran , T. Duguet

Facilitated by a rigorous partitioning of a molecular system's orbital basis into two fundamental subspaces - a reference and an expansion space, both with orbitals of unspecified occupancy - we generalize our recently introduced many-body…

Chemical Physics · Physics 2019-12-12 Janus J. Eriksen , Jürgen Gauss

A systematic method for determining correlated wavefunctions of extended systems in the ground and excited states is presented. It allows to fully exploit the power of quantum-chemical programs designed for correlation calculations of…

Other Condensed Matter · Physics 2007-05-23 V. Bezugly

Trajectories provide dynamical information that is discarded in free energy calculations, for which we sought to design a scheme with the hope of saving cost for generating dynamical information. We first demonstrated that snapshots in a…

Chemical Physics · Physics 2016-08-23 Kai Wang , Shiyang Long , Pu Tian

A new state specific correlation correction to configuration interaction singles (CIS) excitation energies is preseted using coupled cluster perturbation theory (CCPT). General expressions for CIS-CCPT are derived and expanded explicitly to…

Chemical Physics · Physics 2015-06-19 Jason N. Byrd , Victor F. Lotrich , Rodney J. Bartlett