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Title: Molecular hydrogen adsorbed on benzene: Insights from a quantum Monte Carlo study

Abstract

We present a quantum Monte Carlo study of the hydrogen-benzene system where binding is very weak. We demonstrate that the binding is well described at both variational Monte Carlo (VMC) and diffusion Monte Carlo (DMC) levels by a Jastrow correlated single determinant geminal wave function with an optimized compact basis set that includes diffuse orbitals. Agreement between VMC and fixed-node DMC binding energies is found to be within 0.18mhartree, suggesting that the calculations are well converged with respect to the basis. Essentially the same binding is also found in independent DMC calculations using a different trial wave function of a more conventional Slater–Jastrow form, supporting our conclusion that the binding energy is accurate and includes all effects of correlation. Here, we compare with previous calculations, and we discuss the physical mechanisms of the interaction, the role of diffuse basis functions, and the charge redistribution in the bond.

Authors:
 [1];  [1];  [2];  [3];  [1]
+ Show Author Affiliations
  1. Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States)
  2. National Center for Supercomputing Applications, Urbana, IL (United States); Univ. of Illinois at Urbana-Champaign, Urbana, IL (United States)
  3. International School for Advanced Studies, Trieste (Italy); DEMOCRITOS, National Simulation Center, Trieste (Italy)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); UT-Battelle LLC/ORNL, Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1564652
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 129; Journal Issue: 16; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; Physics

Citation Formats

Beaudet, Todd D., Casula, Michele, Kim, Jeongnim, Sorella, Sandro, and Martin, Richard M. Molecular hydrogen adsorbed on benzene: Insights from a quantum Monte Carlo study. United States: N. p., 2008. Web. doi:10.1063/1.2987716.
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Beaudet, Todd D., Casula, Michele, Kim, Jeongnim, Sorella, Sandro, & Martin, Richard M. Molecular hydrogen adsorbed on benzene: Insights from a quantum Monte Carlo study. United States. https://doi.org/10.1063/1.2987716
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Beaudet, Todd D., Casula, Michele, Kim, Jeongnim, Sorella, Sandro, and Martin, Richard M. Tue . "Molecular hydrogen adsorbed on benzene: Insights from a quantum Monte Carlo study". United States. https://doi.org/10.1063/1.2987716. https://www.osti.gov/servlets/purl/1564652.
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@article{osti_1564652,
title = {Molecular hydrogen adsorbed on benzene: Insights from a quantum Monte Carlo study},
author = {Beaudet, Todd D. and Casula, Michele and Kim, Jeongnim and Sorella, Sandro and Martin, Richard M.},
abstractNote = {We present a quantum Monte Carlo study of the hydrogen-benzene system where binding is very weak. We demonstrate that the binding is well described at both variational Monte Carlo (VMC) and diffusion Monte Carlo (DMC) levels by a Jastrow correlated single determinant geminal wave function with an optimized compact basis set that includes diffuse orbitals. Agreement between VMC and fixed-node DMC binding energies is found to be within 0.18mhartree, suggesting that the calculations are well converged with respect to the basis. Essentially the same binding is also found in independent DMC calculations using a different trial wave function of a more conventional Slater–Jastrow form, supporting our conclusion that the binding energy is accurate and includes all effects of correlation. Here, we compare with previous calculations, and we discuss the physical mechanisms of the interaction, the role of diffuse basis functions, and the charge redistribution in the bond.},
doi = {10.1063/1.2987716},
journal = {Journal of Chemical Physics},
number = 16,
volume = 129,
place = {United States},
year = {Tue Oct 28 00:00:00 EDT 2008},
month = {Tue Oct 28 00:00:00 EDT 2008}
}
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https://doi.org/10.1063/1.2987716
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    Works referencing / citing this record:

    Quantum Monte Carlo for noncovalent interactions: an efficient protocol attaining benchmark accuracy
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