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The accuracy and efficiency of ab-initio quantum Monte Carlo (QMC) algorithms benefits greatly from compact variational trial wave functions that accurately reproduce ground state properties of a system. We investigate the possibility of…

Materials Science · Physics 2019-01-30 Shivesh Pathak , Lucas K. Wagner

The dissociation energies of four transition metal dimers are determined using diffusion Monte Carlo. The Jastrow, CI, and molecular orbital parameters of the wave function are both partially and fully optimized with respect to the…

Chemical Physics · Physics 2019-09-06 Jil Ludovicy , Kaveh Haghighi Mood , Arne Lüchow

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

Diffusion quantum Monte Carlo calculations with partial and full optimization of the guide function are carried out for the dissociation of the FeS molecule. For the first time, quantum Monte Carlo orbital optimization for transition metal…

Chemical Physics · Physics 2017-07-31 Kaveh Haghighi Mood , Arne Lüchow

Many quantum many-body wavefunctions, such as Jastrow-Slater, tensor network, and neural quantum states, are studied with the variational Monte Carlo technique, where stochastic optimization is usually performed to obtain a faithful…

Strongly Correlated Electrons · Physics 2025-08-21 Ruojing Peng , Garnet Kin-Lic Chan

In this work, we introduce three algorithmic improvements to reduce the cost and improve the scaling of orbital space variational Monte Carlo (VMC). First, we show that by appropriately screening the one- and two-electron integrals of the…

Chemical Physics · Physics 2018-07-30 Iliya Sabzevari , Sandeep Sharma

Recently, a diffusion Monte Carlo algorithm was applied to the study of spin dependent interactions in condensed matter. Following some of the ideas presented therein, and applied to a Hamiltonian containing a Rashba-like interaction, a…

Strongly Correlated Electrons · Physics 2015-05-27 Alberto Ambrosetti , Pier Luigi Silvestrelli , Flavio Toigo , Lubos Mitas , Francesco Pederiva

A method is developed that allows analysis of quantum Monte Carlo simulations to identify errors in trial wave functions. The purpose of this method is to allow for the systematic improvement of variational wave functions by identifying…

Strongly Correlated Electrons · Physics 2016-08-03 Kiel T. Williams , Lucas K. Wagner

We investigate how the fixed-node diffusion Monte Carlo energy of solids depends on single-particle orbitals used in Slater--Jastrow wave functions. We demonstrate that the dependence can be significant, in particular in the case of 3d…

Materials Science · Physics 2010-09-09 Jindrich Kolorenc , Shuming Hu , Lubos Mitas

We study lithium systems over a range of number of atoms, e.g., atomic anion, dimer, metallic cluster, and body-centered cubic crystal by the diffusion Monte Carlo method. The calculations include both core and valence electrons in order to…

Computational Physics · Physics 2015-07-29 Kevin Rasch , Lubos Mitas

We investigate the inclusion of variable spins in electronic structure quantum Monte Carlo, with a focus on diffusion Monte Carlo with Hamiltonians that include spin-orbit interactions. Following our previous introduction of fixed-phase…

Computational Physics · Physics 2016-07-27 Cody A. Melton , M. Chandler Bennett , Lubos Mitas

This work introduces meta estimators that combine multiple multifidelity techniques based on control variates, importance sampling, and information reuse to yield a quasi-multiplicative amount of variance reduction. The proposed meta…

Computational Physics · Physics 2023-01-19 Frederick Law , Antoine Cerfon , Benjamin Peherstorfer , Florian Wechsung

We present a comparison between a number of recently introduced low-memory wave function optimization methods for variational Monte Carlo in which we find that first and second derivative methods possess strongly complementary relative…

Strongly Correlated Electrons · Physics 2019-07-24 Leon Otis , Eric Neuscamman

Highly flexible Jastrow factors have found significant use in stochastic electronic structure methods such as variational Monte Carlo (VMC) and diffusion Monte Carlo, as well as in quantum chemical transcorrelated (TC) approaches, which…

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

Variational wave functions used in the variational Monte Carlo (VMC) method are extensively improved to overcome the biases coming from the assumed variational form of the wave functions. We construct a highly generalized variational form…

Strongly Correlated Electrons · Physics 2008-10-27 Daisuke Tahara , Masatoshi Imada

The multi-configurational self-consistent field theory is considered the standard starting point for almost all multireference approaches required for strongly-correlated molecular problems. The limitation of the approach is generally given…

Chemical Physics · Physics 2015-10-14 Robert E. Thomas , Qiming Sun , Ali Alavi , George H. Booth

We modify the reweighting factor of the projector used in diffusion Monte Carlo to reduce the time-step error of the total energy. Further, we present a reweighting scheme that has the desirable feature that it is exactly size-consistent,…

Chemical Physics · Physics 2024-03-18 Tyler A. Anderson , Manolo C. Per , C. J. Umrigar

Variational quantum algorithms are poised to have significant impact on high-dimensional optimization, with applications in classical combinatorics, quantum chemistry, and condensed matter. Nevertheless, the optimization landscape of these…

Quantum Physics · Physics 2022-02-02 Taylor L. Patti , Omar Shehab , Khadijeh Najafi , Susanne F. Yelin

Quantum mechanics for many-body systems may be reduced to the evaluation of integrals in 3N dimensions using Monte-Carlo, providing the Quantum Monte Carlo ab initio methods. Here we limit ourselves to expectation values for trial…

Computational Physics · Physics 2010-11-22 John Robert Trail , Ryo Maezono
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