Investigation of a Quantum Monte Carlo Protocol To Achieve High Accuracy and High-Throughput Materials Formation Energies
[1];
- Department of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States
- Department of Materials Science and Engineering, Johns Hopkins University, Baltimore, Maryland 21218, United States
- Department of Physics, University of Illinois at Urbana−Champaign, Urbana−Champaign, Illinois 61801, United States
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.
- Research Organization:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)
- Sponsoring Organization:
- USDOE Office of Science (SC)
- OSTI ID:
- 1565572
- Journal Information:
- Journal of Chemical Theory and Computation, Vol. 13, Issue 5; ISSN 1549-9618
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
Similar Records
Accuracy of DFT computed oxygen-vacancy formation energies and high-throughput search of solar thermochemical water-splitting compounds
Quantifying uncertainty in high-throughput density functional theory: A comparison of AFLOW, Materials Project, and OQMD