Abstract
Pseudopotential locality errors have hampered the applications of the diffusion Monte Carlo (DMC) method in materials containing transition metals, in particular oxides. We have developed locality error free effective core potentials, pseudo-Hamiltonians, for transition metals ranging from Cr to Zn. We have modified a procedure published by some of us in Bennett et al. [J. Chem. Theory Comput. 18, 828 (2022)]. We carefully optimized our pseudo-Hamiltonians and achieved transferability errors comparable to the best semilocal pseudopotentials used with DMC but without incurring in locality errors. Our pseudo-Hamiltonian set (named OPH23) bears the potential to significantly improve the accuracy of many-body-first-principles calculations in fundamental science research of complex materials involving transition metals.
| Original language | English |
|---|---|
| Article number | 164114 |
| Journal | Journal of Chemical Physics |
| Volume | 159 |
| Issue number | 16 |
| DOIs | |
| State | Published - Oct 28 2023 |
Funding
This manuscript has been authored by UT-Battelle, LLC, under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy (DOE). The U.S. government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for U.S. government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). The work in ORNL (T.I., M.C.B., J.T.K., and F.A.R.) was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. K.H. is grateful for financial support from MEXT-KAKENHI, Japan (Grant Nos. JP19K05029, JP21K03400, JP22H02170, and JP23H04623), and the Air Force Office of Scientific Research, United States (Award No. FA2386-22-1-4065). R.M. is grateful for financial supports from MEXT-KAKENHI (Grant Nos. JP22H05146, JP21K03400, and JP19H04692), from the Air Force Office of Scientific Research (AFOSR-AOARD Grant Nos. FA2386-17-1-4049 and FA2386-19-1-4015), and from JSPS Bilateral Joint Projects (Grant No. JPJSBP120197714). An award of computer time was provided by the Innovative and Novel Computational Impact on Theory and Experiment (INCITE) program. This research used computational resources of the Oak Ridge Leadership Computing Facility, which is a DOE Office of Science User Facility supported under Contract No. DE-AC05-00OR22725. This research also used resources of the Research Center for Advanced Computing Infrastructure (RCACI) at JAIST.
| Funders | Funder number |
|---|---|
| AFOSR-AOARD | FA2386-19-1-4015, FA2386-17-1-4049 |
| MEXT-KAKENHI | JP19K05029, JP21K03400, JP23H04623, JP22H02170 |
| U.S. Department of Energy | |
| Air Force Office of Scientific Research | JP19H04692, JP22H05146, FA2386-22-1-4065 |
| Office of Science | DE-AC05-00OR22725 |
| Basic Energy Sciences | |
| Oak Ridge National Laboratory | |
| Division of Materials Sciences and Engineering | |
| Japan Society for the Promotion of Science | JPJSBP120197714 |