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Research output: Contribution to Journal/Magazine › Journal article › peer-review
Research output: Contribution to Journal/Magazine › Journal article › peer-review
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TY - JOUR
T1 - Reproducibility of fixed-node diffusion Monte Carlo across diverse community codes
T2 - The case of water–methane dimer
AU - Della Pia, F
AU - Shi, B. X.
AU - Al-Hamdani, Y. S.
AU - Alfe, D.
AU - Anderson, T. A.
AU - Barborini, M.
AU - Benali, A.
AU - Casula, M.
AU - Drummond, Neil
AU - Dubecky, M.
AU - Filippi, C.
AU - Kent, P. R. C.
AU - Krogel, J. T.
AU - Lopez Rios, P.
AU - Luchow, A
AU - Luo, Y.
AU - Michaelides, A.
AU - Mitas, L.
AU - Nakano, K.
AU - Needs, R. J.
AU - Per, M. C.
AU - Scemama, A.
AU - Schultze, J.
AU - Shinde, R.
AU - Slootman, E.
AU - Sorella, S.
AU - Tkatchenko, A.
AU - Towler, M.
AU - Umrigar, C. J.
AU - Wagner, L. K.
AU - Wheeler, W. A.
AU - Zhou, H.
AU - Zen, A.
PY - 2025/9/8
Y1 - 2025/9/8
N2 - Fixed-node diffusion quantum Monte Carlo (FN-DMC) is a widely trusted many-body method for solving the Schrödinger equation, known for its reliable predictions of material and molecular properties. Furthermore, its excellent scalability with system complexity and near-perfect utilization of computational power make FN-DMC ideally positioned to leverage new advances in computing to address increasingly complex scientific problems. Even though the method is widely used as a computational gold standard, reproducibility across the numerous FN-DMC code implementations has yet to be demonstrated. This difficulty stems from the diverse array of DMC algorithms and trial wave functions, compounded by the method’s inherent stochastic nature. This study represents a community-wide effort to assess the reproducibility of the method, affirming that yes, FN-DMC is reproducible (when handled with care). Using the water–methane dimer as the canonical test case, we compare results from eleven different FN-DMC codes and show that the approximations to treat the non-locality of pseudopotentials are the primary source of the discrepancies between them. In particular, we demonstrate that, for the same choice of determinantal component in the trial wave function, reliable and reproducible predictions can be achieved by employing the T-move, the determinant locality approximation, or the determinant T-move schemes, while the older locality approximation leads to considerable variability in results. These findings demonstrate that, with appropriate choices of algorithmic details, fixed-node DMC is reproducible across diverse community codes—highlighting the maturity and robustness of the method as a tool for open and reliable computational science.
AB - Fixed-node diffusion quantum Monte Carlo (FN-DMC) is a widely trusted many-body method for solving the Schrödinger equation, known for its reliable predictions of material and molecular properties. Furthermore, its excellent scalability with system complexity and near-perfect utilization of computational power make FN-DMC ideally positioned to leverage new advances in computing to address increasingly complex scientific problems. Even though the method is widely used as a computational gold standard, reproducibility across the numerous FN-DMC code implementations has yet to be demonstrated. This difficulty stems from the diverse array of DMC algorithms and trial wave functions, compounded by the method’s inherent stochastic nature. This study represents a community-wide effort to assess the reproducibility of the method, affirming that yes, FN-DMC is reproducible (when handled with care). Using the water–methane dimer as the canonical test case, we compare results from eleven different FN-DMC codes and show that the approximations to treat the non-locality of pseudopotentials are the primary source of the discrepancies between them. In particular, we demonstrate that, for the same choice of determinantal component in the trial wave function, reliable and reproducible predictions can be achieved by employing the T-move, the determinant locality approximation, or the determinant T-move schemes, while the older locality approximation leads to considerable variability in results. These findings demonstrate that, with appropriate choices of algorithmic details, fixed-node DMC is reproducible across diverse community codes—highlighting the maturity and robustness of the method as a tool for open and reliable computational science.
U2 - 10.1063/5.0272974
DO - 10.1063/5.0272974
M3 - Journal article
VL - 163
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
SN - 0021-9606
IS - 10
M1 - 104110
ER -