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Phaseless auxiliary-field quantum Monte Carlo (ph-AFQMC) has emerged as a promising electronic structure method for correlated electronic systems. However, the quality of its predictions depends critically on the choice of trial…

Chemical Physics · Physics 2026-05-06 Don Danilov , Brad Ganoe , Leon Otis , Zhi Gong , Zixiang Lu , James Shee

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…

Chemical Physics · Physics 2025-09-24 Leon Otis , Sri Gudivada , Marvin Friede , James Shee

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…

Chemical Physics · Physics 2022-09-28 Joonho Lee , Hung Q. Pham , David R. Reichman

We extend the use of coupled cluster (CC) trial states in the phaseless auxiliary-field quantum Monte Carlo (AFQMC) method beyond single and double excitations to include both triple and quadruple excitations. With this AFQMC/CC hierarchy,…

Chemical Physics · Physics 2025-10-09 Eirik F. Kjønstad , Yann Damour , Sandeep Sharma , Garnet Kin-Lic Chan

We introduce an efficient approach to implement neural network quantum states (NNQS) as trial wavefunctions in auxiliary-field quantum Monte Carlo (AFQMC). NNQS are a recently developed class of variational ans\"atze capable of flexibly…

Chemical Physics · Physics 2025-10-07 Zhi-Yu Xiao , Bowen Kan , Huan Ma , Bowen Zhao , Honghui Shang

We propose using the wave function generated by the quantum selected configuration interaction (QSCI) method as the trial wave function in phaseless auxiliary-field quantum Monte Carlo (ph-AFQMC). In the QSCI framework, electronic…

In this study, we evaluate multi-configurational trial wave function protocols for phaseless auxiliary field quantum Monte Carlo (ph-AFQMC) on transition metal containing systems. First, we benchmark vertical ionization potentials for 22 3d…

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…

Computational Physics · Physics 2018-09-07 James Shee , Evan J. Arthur , Shiwei Zhang , David R. Reichman , Richard A. Friesner

The accuracy of phaseless auxiliary-field quantum Monte Carlo (ph-AFQMC) can be systematically improved with better trial states. Using multi-Slater determinant trial states, ph-AFQMC has the potential to faithfully treat strongly…

Chemical Physics · Physics 2024-06-13 Yifei Huang , Zhen Guo , Hung Q. Pham , Dingshun Lv

We introduce an efficient approach to implement correlated many-body trial wave functions in auxiliary-field quantum Monte Carlo (AFQMC). To control the sign/phase problem in AFQMC, a constraint is derived from an exact gauge condition but…

Strongly Correlated Electrons · Physics 2025-10-27 Zhi-Yu Xiao , Zixiang Lu , Yixiao Chen , Tao Xiang , Shiwei Zhang

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

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…

Computational Physics · Physics 2020-10-14 Fionn D. Malone , Anouar Benali , Miguel A. Morales , Michel Caffarel , P. R. C. Kent , Luke Shulenburger

We present efficient algorithms for using selected configuration interaction (sCI) trial wave functions in phaseless auxiliary field quantum Monte Carlo (ph-AFQMC). These advancements, geared towards optimizing computational performance for…

Chemical Physics · Physics 2022-05-18 Ankit Mahajan , Joonho Lee , Sandeep Sharma

We investigate the viability of the phaseless finite temperature auxiliary field quantum Monte Carlo (ph-FT-AFQMC) method for ab initio systems using the uniform electron gas as a model. Through comparisons with exact results and finite…

Chemical Physics · Physics 2021-02-15 Joonho Lee , Miguel A. Morales , Fionn D. Malone

We explore different ways of incorporating accurate trial wave functions into free projection auxiliary field quantum Monte Carlo (fp-AFQMC). Trial states employed include coupled cluster singles and doubles, multi-Slater, and symmetry…

Chemical Physics · Physics 2021-04-15 Ankit Mahajan , Sandeep Sharma

We present phaseless auxiliary-field (AF) quantum Monte Carlo (QMC) calculations of the ground states of some hydrogen-bonded systems. These systems were selected to test and benchmark different aspects of the new phaseless AF QMC method.…

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

Phaseless Auxiliary-Field Quantum Monte Carlo (ph-AFQMC) has recently emerged as a promising method for the production of benchmark-level simulations of medium to large-sized molecules, due to its accuracy and favorable polynomial scaling…

In this work, we develop a size extensive Auxiliary-Field Quantum Monte Carlo (AFQMC) approach that scales as $O(N^5)$ for local energy evaluation by treating the Coupled Cluster Singles and Doubles (CCSD) trial wavefunctions…

Chemical Physics · Physics 2026-05-13 Yichi Zhang , Ankit Mahajan , Yann Damour , Sandeep Sharma

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

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…

Computational Physics · Physics 2013-07-09 Wirawan Purwanto , Shiwei Zhang , Henry Krakauer
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