Reproducibility of fixed-node diffusion Monte Carlo across diverse community codes : The case of water–methane dimer

Della Pia, F and Shi, B. X. and Al-Hamdani, Y. S. and Alfe, D. and Anderson, T. A. and Barborini, M. and Benali, A. and Casula, M. and Drummond, Neil and Dubecky, M. and Filippi, C. and Kent, P. R. C. and Krogel, J. T. and Lopez Rios, P. and Luchow, A and Luo, Y. and Michaelides, A. and Mitas, L. and Nakano, K. and Needs, R. J. and Per, M. C. and Scemama, A. and Schultze, J. and Shinde, R. and Slootman, E. and Sorella, S. and Tkatchenko, A. and Towler, M. and Umrigar, C. J. and Wagner, L. K. and Wheeler, W. A. and Zhou, H. and Zen, A. (2025) Reproducibility of fixed-node diffusion Monte Carlo across diverse community codes : The case of water–methane dimer. Journal of Chemical Physics, 163 (10): 104110. ISSN 0021-9606

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Abstract

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.