TY - UNPB
T1 - Is fixed-node diffusion quantum Monte Carlo reproducible?
AU - Pia, Flaviano Della
AU - Shi, Benjamin
AU - Al-Hamdani, Yasmine S.
AU - Alfè, Dario
AU - Anderson, Tyler
AU - Barborini, Matteo
AU - Benali, Anouar
AU - Casula, Michele
AU - Drummond, Neil
AU - Dubecký, Matúš
AU - Filippi, Claudia
AU - Kent, Paul
AU - Krogel, Jaron
AU - López Ríos, Pablo
AU - Lüchow, Arne
AU - Luo, Ye
AU - Michaelides, Angelos
AU - Mitas, Lubos
AU - Nakano, Kosuke
AU - Needs, Richard
AU - Per, Manolo
AU - Scemama, Anthony
AU - Schultze, Jil
AU - Shinde, Ravindra
AU - Slootman, Emiel
AU - Sorella, Sandro
AU - Tkatchenko, Alexandre
AU - Towler, Mike
AU - Umrigar, Cyrus
AU - Wagner, Lucas
AU - Wheeler, William Ashwin
AU - Zhou, Haihan
AU - Zen, Andrea
PY - 2025/1/22
Y1 - 2025/1/22
N2 - 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.
AB - 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.
KW - physics.comp-ph
KW - cond-mat.mtrl-sci
KW - physics.chem-ph
U2 - 10.48550/arXiv.2501.12950
DO - 10.48550/arXiv.2501.12950
M3 - Preprint
BT - Is fixed-node diffusion quantum Monte Carlo reproducible?
PB - ArXiv.org
ER -