Is fixed-node diffusion quantum Monte Carlo reproducible?

Flaviano Della Pia, Benjamin Shi, Yasmine S. Al-Hamdani, Dario Alfè, Tyler Anderson, Matteo Barborini, Anouar Benali, Michele Casula, Neil Drummond, Matúš Dubecký, Claudia Filippi, Paul Kent, Jaron Krogel, Pablo López Ríos, Arne Lüchow, Ye Luo, Angelos Michaelides, Lubos Mitas, Kosuke Nakano, Richard NeedsManolo Per, Anthony Scemama, Jil Schultze, Ravindra Shinde, Emiel Slootman, Sandro Sorella, Alexandre Tkatchenko, Mike Towler, Cyrus Umrigar, Lucas Wagner, William Ashwin Wheeler, Haihan Zhou, Andrea Zen

Research output: Working paperPreprintAcademic

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Abstract

Fixed-node diffusion quantum Monte Carlo (FN-DMC) is a widely-trusted many-body method for solving the Schr\"{o}dinger 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 makes 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 address the titular question, 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 (TM), the determinant locality approximation (DLA), or the determinant T-move (DTM) schemes, while the older locality approximation (LA) leads to considerable variability in results. This work lays the foundation to establish accurate and reproducible FN-DMC estimates for all future studies across applications in materials science, physics, chemistry, and biology.
Original languageEnglish
PublisherArXiv.org
DOIs
Publication statusPublished - 22 Jan 2025

Keywords

  • physics.comp-ph
  • cond-mat.mtrl-sci
  • physics.chem-ph

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