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Title: Benchmarking the pseudopotential and fixed-node approximations in diffusion Monte Carlo calculations of molecules and solids

We performed diffusion Monte Carlo (DMC) calculations of the spectroscopic properties of a large set of molecules, assessing the effect of different approximations. In systems containing elements with large atomic numbers, we show that the errors associated with the use of nonlocal mean-field-based pseudopotentials in DMC calculations can be significant and may surpass the fixed-node error. In conclusion, we suggest practical guidelines for reducing these pseudopotential errors, which allow us to obtain DMC-computed spectroscopic parameters of molecules and equation of state properties of solids in excellent agreement with experiment.
Authors:
 [1] ;  [2] ;  [1] ;  [1]
  1. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Publication Date:
Report Number(s):
LLNL-JRNL-676682
Journal ID: ISSN 2469-9950; KC0202030; ERKCK03
Grant/Contract Number:
AC05-00OR22725; AC52-07NA27344; AC04-94AL85000; LDRD 13- ERD-067
Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 93; Journal Issue: 9; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 74 ATOMIC AND MOLECULAR PHYSICS; 36 MATERIALS SCIENCE
OSTI Identifier:
1261352
Alternate Identifier(s):
OSTI ID: 1244158; OSTI ID: 1262188

Nazarov, Roman, Shulenburger, Luke, Morales, Miguel A., and Hood, Randolph Q.. Benchmarking the pseudopotential and fixed-node approximations in diffusion Monte Carlo calculations of molecules and solids. United States: N. p., Web. doi:10.1103/PhysRevB.93.094111.
Nazarov, Roman, Shulenburger, Luke, Morales, Miguel A., & Hood, Randolph Q.. Benchmarking the pseudopotential and fixed-node approximations in diffusion Monte Carlo calculations of molecules and solids. United States. doi:10.1103/PhysRevB.93.094111.
Nazarov, Roman, Shulenburger, Luke, Morales, Miguel A., and Hood, Randolph Q.. 2016. "Benchmarking the pseudopotential and fixed-node approximations in diffusion Monte Carlo calculations of molecules and solids". United States. doi:10.1103/PhysRevB.93.094111. https://www.osti.gov/servlets/purl/1261352.
@article{osti_1261352,
title = {Benchmarking the pseudopotential and fixed-node approximations in diffusion Monte Carlo calculations of molecules and solids},
author = {Nazarov, Roman and Shulenburger, Luke and Morales, Miguel A. and Hood, Randolph Q.},
abstractNote = {We performed diffusion Monte Carlo (DMC) calculations of the spectroscopic properties of a large set of molecules, assessing the effect of different approximations. In systems containing elements with large atomic numbers, we show that the errors associated with the use of nonlocal mean-field-based pseudopotentials in DMC calculations can be significant and may surpass the fixed-node error. In conclusion, we suggest practical guidelines for reducing these pseudopotential errors, which allow us to obtain DMC-computed spectroscopic parameters of molecules and equation of state properties of solids in excellent agreement with experiment.},
doi = {10.1103/PhysRevB.93.094111},
journal = {Physical Review B},
number = 9,
volume = 93,
place = {United States},
year = {2016},
month = {3}
}