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Title: Fast and accurate quantum Monte Carlo for molecular crystals

Abstract

Computer simulation plays a central role in modern-day materials science. The utility of a given computational approach depends largely on the balance it provides between accuracy and computational cost. Molecular crystals are a class of materials of great technological importance which are challenging for even the most sophisticated ab initio electronic structure theories to accurately describe. This is partly because they are held together by a balance of weak intermolecular forces but also because the primitive cells of molecular crystals are often substantially larger than those of atomic solids. Here, we demonstrate that diffusion quantum Monte Carlo (DMC) delivers subchemical accuracy for a diverse set of molecular crystals at a surprisingly moderate computational cost. As such, we anticipate that DMC can play an important role in understanding and predicting the properties of a large number of molecular crystals, including those built from relatively large molecules which are far beyond reach of other high-accuracy methods.

Authors:
 [1]; ORCiD logo [1];  [2];  [3];  [4];  [1]
  1. Univ. College London (United Kingdom). Dept. of Physics and Astronomy, Thomas Young Centre and London Centre for Nanotechnology
  2. Academy of Sciences of the Czech Republic, Prague (Czech Republic). J. Heyrovsky Inst. of Physical Chemistry; Charles Univ., Prague (Czech Republic). Dept. of Chemical Physics and Optics
  3. Univ. of Luxembourg (Luxembourg). Physics and Material Science Research Unit
  4. Univ. College London (United Kingdom). Thomas Young Centre and London Centre for Nanotechnology; Univ. College London (United Kingdom). Dept. of Earth Sciences
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); UT-Battelle LLC/ORNL, Oak Ridge, TN (Unted States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1565681
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 115; Journal Issue: 8; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Science & Technology

Citation Formats

Zen, Andrea, Brandenburg, Jan Gerit, Klimeš, Jiří, Tkatchenko, Alexandre, Alfè, Dario, and Michaelides, Angelos. Fast and accurate quantum Monte Carlo for molecular crystals. United States: N. p., 2018. Web. doi:10.1073/pnas.1715434115.
Zen, Andrea, Brandenburg, Jan Gerit, Klimeš, Jiří, Tkatchenko, Alexandre, Alfè, Dario, & Michaelides, Angelos. Fast and accurate quantum Monte Carlo for molecular crystals. United States. doi:10.1073/pnas.1715434115.
Zen, Andrea, Brandenburg, Jan Gerit, Klimeš, Jiří, Tkatchenko, Alexandre, Alfè, Dario, and Michaelides, Angelos. Mon . "Fast and accurate quantum Monte Carlo for molecular crystals". United States. doi:10.1073/pnas.1715434115. https://www.osti.gov/servlets/purl/1565681.
@article{osti_1565681,
title = {Fast and accurate quantum Monte Carlo for molecular crystals},
author = {Zen, Andrea and Brandenburg, Jan Gerit and Klimeš, Jiří and Tkatchenko, Alexandre and Alfè, Dario and Michaelides, Angelos},
abstractNote = {Computer simulation plays a central role in modern-day materials science. The utility of a given computational approach depends largely on the balance it provides between accuracy and computational cost. Molecular crystals are a class of materials of great technological importance which are challenging for even the most sophisticated ab initio electronic structure theories to accurately describe. This is partly because they are held together by a balance of weak intermolecular forces but also because the primitive cells of molecular crystals are often substantially larger than those of atomic solids. Here, we demonstrate that diffusion quantum Monte Carlo (DMC) delivers subchemical accuracy for a diverse set of molecular crystals at a surprisingly moderate computational cost. As such, we anticipate that DMC can play an important role in understanding and predicting the properties of a large number of molecular crystals, including those built from relatively large molecules which are far beyond reach of other high-accuracy methods.},
doi = {10.1073/pnas.1715434115},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 8,
volume = 115,
place = {United States},
year = {2018},
month = {2}
}

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Cited by: 17 works
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