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We extend correlated sampling from classical auxiliary-field quantum Monte Carlo to the quantum-classical (QC-AFQMC) framework, enabling accurate nuclear force computations crucial for geometry optimization and reaction dynamics. Stochastic…

Auxiliary Field Quantum Monte Carlo (AFQMC) has emerged as a powerful framework for treating strongly correlated electronic systems, offering a favorable balance between computational cost and accuracy. In this paper, we present a novel…

化学物理 · 物理学 2026-04-03 Maxine Luo , Victor Chen , Yu Wang , Christian B. Mendl

The auxiliary-field quantum Monte Carlo (AFQMC) method is a general numerical method for correlated many-electron systems, which is being increasingly applied in lattice models, atoms, molecules, and solids. Here we introduce the theory and…

计算物理 · 物理学 2021-02-24 Hao Shi , Shiwei Zhang

The auxiliary-field quantum Monte Carlo (AFQMC) method provides a computational framework for solving the time-independent Schroedinger equation in atoms, molecules, solids, and a variety of model systems. AFQMC has recently witnessed…

计算物理 · 物理学 2018-08-14 Mario Motta , Shiwei Zhang

To make useful connections with experimental measurements, correlated electronic structure theories must accurately predict chemical properties in addition to energies. We present a finite-difference based algorithm to compute first-order…

化学物理 · 物理学 2025-09-24 Leon Otis , Sri Gudivada , Marvin Friede , James Shee

The bond dissociation energies of a set of 44 3d transition metal-containing diatomics are computed with phaseless auxiliary-field quantum Monte Carlo (ph-AFQMC) utilizing a correlated sampling technique. We investigate molecules with H, N,…

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…

化学物理 · 物理学 2024-02-09 Z. Sukurma , M. Schlipf , M. Humer , A. Taheridehkordi , G. Kresse

In this work, we present an overview of the phaseless auxiliary-field quantum Monte Carlo (ph- AFQMC) approach from a computational quantum chemistry perspective, and present a numerical assessment of its performance on main group chemistry…

化学物理 · 物理学 2022-09-28 Joonho Lee , Hung Q. Pham , David R. Reichman

In the last few years we have been developing a Monte Carlo simulation method to cope with systems of many electrons and ions in the Born-Oppenheimer (BO) approximation, the Coupled Electron-Ion Monte Carlo Method (CEIMC). Electronic…

计算物理 · 物理学 2007-05-23 Carlo Pierleoni , David M. Ceperley

We develop a local correlation variant of auxiliary field quantum Monte Carlo (AFQMC) that is based on local natural orbitals (LNO-AFQMC). In LNO-AFQMC, independent AFQMC calculations are performed for each localized occupied orbital using…

化学物理 · 物理学 2023-08-25 Jo S. Kurian , Hong-Zhou Ye , Ankit Mahajan , Timothy C. Berkelbach , Sandeep Sharma

We present an implementation of phaseless Auxiliary-Field Quantum Monte Carlo (ph-AFQMC) utilizing graphical processing units (GPUs). The AFQMC method is recast in terms of matrix operations which are spread across thousands of processing…

计算物理 · 物理学 2018-09-07 James Shee , Evan J. Arthur , Shiwei Zhang , David R. Reichman , Richard A. Friesner

The Auxiliary-Field Quantum Monte Carlo (AFQMC) algorithm is a powerful quantum many-body method that can be used successfully as an alternative to standard quantum chemistry approaches to compute the ground state of many body systems, such…

化学物理 · 物理学 2018-07-23 Edgar Josué Landinez Borda , John A. Gomez , Miguel A. Morales

Recent progress in simulation methodologies and in computer power allow first principle simulations of condensed systems with Born-Oppenheimer electronic energies obtained by Quantum Monte Carlo methods. Computing free energies and…

统计力学 · 物理学 2015-05-30 Elisa Liberatore , Miguel A. Morales , David M. Ceperley , Carlo Pierleoni

Quantum Monte Carlo (QMC) methods are some of the most accurate methods for simulating correlated electronic systems. We investigate the compatibility, strengths and weaknesses of two such methods, namely, diffusion Monte Carlo (DMC) and…

In order to find the equilibrium geometries of molecules and solids and to perform ab initio molecular dynamics, it is necessary to calculate the forces on the nuclei. We present a correlated sampling method to efficiently calculate…

凝聚态物理 · 物理学 2009-10-31 Claudia Filippi , C. J. Umrigar

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.…

量子物理 · 物理学 2024-09-16 Matthew Kiser , Matthias Beuerle , Fedor Simkovic

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…

化学物理 · 物理学 2025-03-04 Lukas Weber , Leonardo dos Anjos Cunha , Miguel A. Morales , Angel Rubio , Shiwei Zhang

We show that the recently developed phaseless auxiliary-field quantum Monte Carlo (AFQMC) method can be used to study excited states, providing an alternative to standard quantum chemistry methods. The phaseless AFQMC approach, whose…

计算物理 · 物理学 2013-07-09 Wirawan Purwanto , Shiwei Zhang , Henry Krakauer

For optimal accuracy, auxiliary-field quantum Monte Carlo (AFQMC) requires trial states consisting of multiple Slater determinants. We develop an efficient algorithm to select the determinants from an AFQMC random walk eliminating the need…

化学物理 · 物理学 2025-07-08 Zoran Sukurma , Martin Schlipf , Georg Kresse

In this work, we test a recently developed method to enhance classical auxiliary-field quantum Monte Carlo (AFQMC) calculations with quantum computers against examples from chemistry and material science, representatives of classes of…

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