Twenty Years of Auxiliary-Field Quantum Monte Carlo in Quantum Chemistry: An Overview and Assessment on Main Group Chemistry and Bond-Breaking

• URL: http://arxiv.org/abs/2208.01280v2
• Date: Tue, 27 Sep 2022 17:09:37 GMT
• Title: Twenty Years of Auxiliary-Field Quantum Monte Carlo in Quantum Chemistry: An Overview and Assessment on Main Group Chemistry and Bond-Breaking
• Abstract summary: We present an overview of the phaseless auxiliary-field quantum Monte Carlo approach from a computational quantum chemistry perspective. We present a numerical assessment of its performance on main group chemistry and bond-breaking problems with a total of 1004 relative energies.
• Score: 0.6445605125467573
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: 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 and bond-breaking problems with a total of 1004 relative energies. While our benchmark study is somewhat limited, we make recommendations for the use of ph-AFQMC for general main-group chemistry applications. For systems where single determinant wave functions are qualitatively accurate, we expect the accuracy of ph-AFQMC in conjunction with a single determinant trial wave function to be between that of coupled-cluster with singles and doubles (CCSD) and CCSD with perturbative triples (CCSD(T)). For these applications, ph-AFQMC should be a method of choice when canonical CCSD(T) is too expensive to run. For systems where multi-reference (MR) wave functions are needed for qualitative accuracy, ph-AFQMC is far more accurate than MR perturbation theory methods and competitive with MR configuration interaction (MRCI) methods. Due to the computational efficiency of ph-AFQMC compared to MRCI, we recommended ph-AFQMC as a method of choice for handling dynamic correlation in MR problems. We conclude with a discussion of important directions for future development of the ph-AFQMC approach.

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