Investigation of a Quantum Monte Carlo Protocol To Achieve High Accuracy and High-Throughput Materials Formation Energies
Author(s)Saritas, Kayahan; Mueller, Tim; Wagner, Lucas; Grossman, Jeffrey C.
MetadataShow full item record
High-throughput calculations based on density functional theory (DFT) methods have been widely implemented in the scientific community. However, depending on both the properties of interest as well as particular chemical/structural phase space, accuracy even for correct trends remains a key challenge for DFT. In this work, we evaluate the use of quantum Monte Carlo (QMC) to calculate material formation energies in a high-throughput environment. We test the performance of automated QMC calculations on 21 compounds with high quality reference data from the Committee on Data for Science and Technology (CODATA) thermodynamic database. We compare our approach to different DFT methods as well as different pseudopotentials, showing that errors in QMC calculations can be progressively improved especially when correct pseudopotentials are used. We determine a set of accurate pseudopotentials in QMC via a systematic investigation of multiple available pseudopotential libraries. We show that using this simple automated recipe, QMC calculations can outperform DFT calculations over a wide set of materials. Out of 21 compounds tested, chemical accuracy has been obtained in formation energies of 11 structures using our QMC recipe, compared to none using DFT calculations.
DepartmentMassachusetts Institute of Technology. Department of Materials Science and Engineering
Journal of Chemical Theory and Computation
American Chemical Society (ACS)
Saritas, Kayahan et al. “Investigation of a Quantum Monte Carlo Protocol To Achieve High Accuracy and High-Throughput Materials Formation Energies.” Journal of Chemical Theory and Computation 13, 5 (April 2017): 1943–1951 © 2017 American Chemical Society
Author's final manuscript