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We report a scalable Fortran implementation of the phaseless auxiliary-field quantum Monte Carlo (ph-AFQMC) and demonstrate its excellent performance and beneficial scaling with respect to system size. Furthermore, we investigate…

Chemical Physics · Physics 2024-02-09 Z. Sukurma , M. Schlipf , M. Humer , A. Taheridehkordi , G. Kresse

Spin-orbit coupling (SOC) is incorporated into the phaseless plane-wave-based auxiliary-field quantum Monte Carlo (pw-AFQMC) method. This integration is implemented using optimized multiple-projector norm-conserving pseudopotentials, which…

Materials Science · Physics 2026-02-13 Zheng Liu , Shiwei Zhang , Fengjie Ma

We present a method for calculating first-order response properties in phaseless auxiliary field quantum Monte Carlo (AFQMC) through the application of automatic differentiation (AD). Biases and statistical efficiency of the resulting…

Chemical Physics · Physics 2023-08-11 Ankit Mahajan , Jo S. Kurian , Joonho Lee , David R. Reichman , Sandeep Sharma

We formulate and characterize a new constraint for Auxiliary Field Quantum Monte Carlo (AFQMC) applicable for general fermionic systems, which allows for the accumulation of phase in the random walk but disallows walkers with a magnitude of…

Chemical Physics · Physics 2023-06-16 John L. Weber , Hung Vuong , Richard A. Friesner , David R. Reichman

We expand upon the recent semi-stochastic adaptation to full configuration interaction quantum Monte Carlo (FCIQMC). We present an alternate method for generating the deterministic space without a priori knowledge of the wave function and…

Computational Physics · Physics 2015-11-17 N. S. Blunt , Simon D. Smart , J. A. F. Kersten , J. S. Spencer , George H. Booth , Ali Alavi

We explore the use in quantum Monte Carlo (QMC) of trial wave functions consisting of a Jastrow factor multiplied by a truncated configuration-interaction (CI) expansion in Slater determinants obtained from a CI perturbatively selected…

Chemical Physics · Physics 2016-01-25 Emmanuel Giner , Roland Assaraf , Julien Toulouse

We present three distinct examples where phaseless auxiliary-field Quantum Monte Carlo (ph-AFQMC) can be reliably performed with a single-determinant trial wavefunction with essential symmetry breaking. We first utilized essential…

Chemical Physics · Physics 2020-04-20 Joonho Lee , Fionn D. Malone , Miguel A. Morales

Phaseless auxiliary-field quantum Monte Carlo (AFQMC) has in several cases been found to perform well on strongly correlated systems. Here, we benchmark the method for three iron-sulfur clusters ([2Fe-2S], [4Fe-4S], and the FeMo cofactor)…

Chemical Physics · Physics 2026-05-06 Eirik F. Kjønstad , Huanchen Zhai , James Shee , Sandeep Sharma , Garnet Kin-Lic Chan

In this article, we present a method for computing accurate and scalable nuclear forces within the phaseless auxiliary-field quantum Monte Carlo (AFQMC) framework. Our approach leverages automatic differentiation of the energy functional to…

Chemical Physics · Physics 2026-02-16 Jo S. Kurian , Ankit Mahajan , Sandeep Sharma

We extend the recently introduced phaseless auxiliary-field quantum Monte Carlo (QMC) approach to any single-particle basis, and apply it to molecular systems with Gaussian basis sets. QMC methods in general scale favorably with system…

Computational Physics · Physics 2007-05-23 W. A. Al-Saidi , Shiwei Zhang , Henry Krakauer

We systematically investigate the calculation of excited states in quantum chemistry using auxiliary field quantum Monte Carlo (AFQMC). Symmetry allows targeting of the lowest triplet excited states in AFQMC based on restricted open-shell…

Chemical Physics · Physics 2025-09-16 Ankit Mahajan , Sandeep Sharma , Shiwei Zhang , David R. Reichman

Using trial wavefunctions prepared on quantum devices to reduce the bias of auxiliary-field quantum Monte Carlo (QC-AFQMC) has established itself as a promising hybrid approach to the simulation of strongly correlated many body systems.…

Quantum Physics · Physics 2024-09-16 Matthew Kiser , Matthias Beuerle , Fedor Simkovic

We introduce a black-box auxiliary field quantum Monte Carlo (AFQMC) approach to perform highly accurate electronic structure calculations using configuration interaction singles and doubles (CISD) trial states. This method consistently…

The computational demand posed by applying multi-Slater determinant trials in phaseless auxiliary-field quantum Monte Carlo methods (MSD-AFQMC) is particularly significant for molecules exhibiting strong correlations. Here, we propose using…

Chemical Physics · Physics 2023-12-27 Hung Q. Pham , Runsheng Ouyang , Dingshun Lv

Model space quantum Monte Carlo (MSQMC) is an extension of full configuration interaction QMC (FCIQMC) that allows us to calculate quasi-degenerate and excited electronic states by sampling the effective Hamiltonian in the model space. We…

Chemical Physics · Physics 2017-12-29 Seiichiro L. Ten-no

We present a generalization of the phaseless auxiliary-field quantum Monte Carlo (AFQMC) method to cavity quantum-electrodynamical (QED) matter systems. The method can be formulated in both the Coulomb and the dipole gauge. We verify its…

Chemical Physics · Physics 2025-03-04 Lukas Weber , Leonardo dos Anjos Cunha , Miguel A. Morales , Angel Rubio , Shiwei Zhang

We marry tensor network states (TNS) and projector quantum Monte Carlo (PMC) to overcome the high computational scaling of TNS and the sign problem of PMC. Using TNS as trial wavefunctions provides a route to systematically improve the sign…

Strongly Correlated Electrons · Physics 2014-07-04 Sebastian Wouters , Brecht Verstichel , Dimitri Van Neck , Garnet Kin-Lic Chan

In diffusion Monte Carlo (DMC) methods, the nodes (or zeroes) of the trial wave function dictate the magnitude of the fixed-node (FN) error. Within standard DMC implementations, they emanate from short multideterminant expansions,…

Chemical Physics · Physics 2018-05-31 Anthony Scemama , Yann Garniron , Michel Caffarel , Pierre-François Loos

We extend the scope of full configuration interaction quantum Monte Carlo (FCIQMC) to be applied to coupled fermion-boson hamiltonians, alleviating the a priori truncation in boson occupation which is necessary for many other wave function…

Strongly Correlated Electrons · Physics 2022-11-09 Robert J. Anderson , Charles C. J. Scott , George H. Booth

Bond stretching mimics different levels of electron correlation and provides a challenging testbed for approximate many-body computational methods. Using the recently developed phaseless auxiliary-field quantum Monte Carlo (AF QMC) method,…

Computational Physics · Physics 2007-10-10 W. A. Al-Saidi , Shiwei Zhang , Henry Krakauer