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A quantum Monte Carlo method of determining Jastrow-Slater wave functions for which the energy is stationary with respect to variations in the single-particle orbitals is presented. A potential is determined by a least-squares fitting of…

Condensed Matter · Physics 2007-05-23 Stephen Fahy , Claudia Filippi

We study three wave function optimization methods based on energy minimization in a variational Monte Carlo framework: the Newton, linear and perturbative methods. In the Newton method, the parameter variations are calculated from the…

Chemical Physics · Physics 2015-06-26 Julien Toulouse , C. J. Umrigar

The number of resident space objects is rising at an alarming rate. Mega-constellations and breakup events are proliferating in most orbital regimes, and safe navigation is becoming increasingly problematic. It is important to be able to…

Instrumentation and Methods for Astrophysics · Physics 2025-04-11 Yannick Sztamfater Garcia , Joaquin Miguez , Manuel Sanjurjo-Rivo

In this work we extend the framework of monotone dynamical systems to a broad and important class of stochastic equations, namely cooperative McKean-Vlasov SDEs with multiplicative noise. Under a locally dissipative assumption, our main…

Probability · Mathematics 2026-01-06 Chunlin Liu , Baoyou Qu , Jinxiang Yao , Yanpeng Zhi

A quantum Monte Carlo method is presented for determining multi-determinantal Jastrow-Slater wave functions for which the energy is stationary with respect to the simultaneous optimization of orbitals and configuration interaction…

Other Condensed Matter · Physics 2009-11-10 Friedemann Schautz , Claudia Filippi

Although self-consistent multi-configuration methods have been used for decades to address the description of atomic and molecular many-body systems, only a few trials have been made in the context of nuclear structure. This work aims at…

Nuclear Theory · Physics 2016-02-02 C. Robin , N. Pillet , D. Peña Arteaga , J. -F. Berger

We present the fully general time-dependent multiconfiguration self-consistent-field method to describe the dynamics of a system consisting of arbitrary different kinds and numbers of interacting fermions and bosons. The total wave function…

Atomic Physics · Physics 2017-10-11 Ryoji Anzaki , Takeshi Sato , Kenichi L. Ishikawa

Natural orbital functional (NOF) theory offers a promising approach for studying strongly correlated systems at an affordable computational cost, with an accuracy comparable to highly demanding wavefunction-based methods. However, its…

Strongly Correlated Electrons · Physics 2025-01-31 Juan Felipe Huan Lew-Yee , Jorge M. del Campo , Mario Piris

Hybrid multiscale modelling has emerged as a useful framework for modelling complex biological phenomena. However, when accounting for stochasticity in the internal dynamics of agents, these models frequently become computationally…

Quantitative Methods · Quantitative Biology 2021-05-11 Daria Stepanova , Helen M. Byrne , Philip K. Maini , Tomás Alarcón

Within Full Configuration Interaction Quantum Monte Carlo, we investigate how the statistical error behaves as a function of the parameters which control the stochastic sampling. We define the inefficiency as a measure of the statistical…

Chemical Physics · Physics 2016-03-15 W. A. Vigor , J. S. Spencer , M. J. Bearpark , A. J. W. Thom

Tailoring the performance of next-generation high entropy materials requires a deep understanding of the competition between entropy-driven random solid solution and enthalpy-driven chemical ordering. Investigating such order and disorder…

Materials Science · Physics 2026-03-24 Fanli Zhou , Hao Chen , Pengxiang Xu , Kai Yang , Zongrui Pei , Xianglin Liu

A reliable and efficient computation of the entire single-particle spectrum of correlated molecules is an outstanding challenge in the field of quantum chemistry, with standard density functional theory approaches often giving an inadequate…

Chemical Physics · Physics 2021-10-08 Oliver J. Backhouse , Alejandro Santana-Bonilla , George H. Booth

The general procedure underlying Hartree-Fock and Kohn-Sham density functional theory calculations consists in optimizing orbitals for a self-consistent solution of the Roothaan-Hall equations in an iterative process. It is often ignored…

Chemical Physics · Physics 2017-03-16 Alain C. Vaucher , Markus Reiher

Stochastic gradient methods are scalable for solving large-scale optimization problems that involve empirical expectations of loss functions. Existing results mainly apply to optimization problems where the objectives are one- or two-level…

Optimization and Control · Mathematics 2018-01-15 Shuoguang Yang , Mengdi Wang , Ethan X. Fang

Approximate natural orbitals are investigated as a way to improve a Monte Carlo configuration interaction (MCCI) calculation. We introduce a way to approximate the natural orbitals in MCCI and test these and approximate natural orbitals…

Chemical Physics · Physics 2013-04-12 J. P. Coe , M. J. Paterson

This paper generalizes stochastic collocation methods to handle correlated non-Gaussian random parameters. The key challenge is to perform a multivariate numerical integration in a correlated parameter space when computing the coefficient…

Numerical Analysis · Computer Science 2018-08-28 Chunfeng Cui , Zheng Zhang

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…

Chemical Physics · Physics 2016-02-02 Ruth S. T. Franklin , James S. Spencer , Alberto Zoccante , Alex J. W. Thom

In order for methods combining ab initio density-functional theory and many-body techniques to become routinely used, a flexible, fast, and easy-to-use implementation is crucial. We present an implementation of a general charge…

Fragmentation methods applied to multireference wave functions constitute a road towards the application of highly accurate ab initio wave function calculations to large molecules and solids. However, it is important for reproducibility and…

Chemical Physics · Physics 2020-07-23 Matthew R. Hermes , Laura Gagliardi

The simultaneous treatment of static and dynamical correlations in strongly-correlated electron systems is a critical challenge. In particular, finding a universal scheme for identifying a single-particle orbital basis that minimizes the…

Quantum Physics · Physics 2024-08-07 Ke Liao , Lexin Ding , Christian Schilling