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Title: Properties of the water to boron nitride interaction: From zero to two dimensions with benchmark accuracy

Abstract

Molecular adsorption on surfaces plays an important part in catalysis, corrosion, desalination, and various other processes that are relevant to industry and in nature. As a complement to experiments, accurate adsorption energies can be obtained using various sophisticated electronic structure methods that can now be applied to periodic systems. The adsorption energy of water on boron nitride substrates, going from zero to 2-dimensional periodicity, is particularly interesting as it calls for an accurate treatment of polarizable electrostatics and dispersion interactions, as well as posing a practical challenge to experiments and electronic structure methods. Here, we present reference adsorption energies, static polarizabilities, and dynamic polarizabilities, for water on BN substrates of varying size and dimension. Adsorption energies are computed with coupled cluster theory, fixed-node quantum Monte Carlo (FNQMC), the random phase approximation, and second order Møller-Plesset theory. These wavefunction based correlated methods are found to agree in molecular as well as periodic systems. The best estimate of the water/h-BN adsorption energy is -107 ± 7 meV from FNQMC. In addition, the water adsorption energy on the BN substrates could be expected to grow monotonically with the size of the substrate due to increased dispersion interactions, but interestingly, this is not themore » case here. This peculiar finding is explained using the static polarizabilities and molecular dispersion coefficients of the systems, as computed from time-dependent density functional theory (DFT). Dynamic as well as static polarizabilities are found to be highly anisotropic in these systems. Finally, the many-body dispersion method in DFT emerges as a particularly useful estimation of finite size effects for other expensive, many-body wavefunction based methods.« less

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [5];  [6]; ORCiD logo [7]; ORCiD logo [5];  [4];  [8]; ORCiD logo [7]
  1. Thomas Young Centre and London Centre for Nanotechnology (United Kingdom); Univ. of Luxembourg (Luxembourg). Physics and Materials Science Research Unit
  2. Max-Planck Society, Berlin (Germany). Fritz Haber Inst.
  3. Thomas Young Centre and London Centre for Nanotechnology (United Kingdom); Univ. College London (United Kingdom). Dept. of Earth Sciences
  4. Max-Planck Inst. for Solid State Research, Stuttgart (Germany)
  5. Univ. of Vienna, Wien (Austria). Faculty of Physics, and Center for Computational Materials Sciences
  6. Thomas Young Centre and London Centre for Nanotechnology (United Kingdom); Univ. College London (United Kingdom). Dept. of Physics and Astronomy, and Dept. of Chemistry
  7. Thomas Young Centre and London Centre for Nanotechnology (United Kingdom); Univ. College London (United Kingdom). Dept. of Physics and Astronomy
  8. Univ. of Luxembourg (Luxembourg). Physics and Materials Science Research Unit
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States); UT-Battelle LLC/ORNL, Oak Ridge, TN (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1565595
Alternate Identifier(s):
OSTI ID: 1373330
Grant/Contract Number:  
AC02-06CH11357; AC05-00OR22725
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 147; Journal Issue: 4; 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

Al-Hamdani, Yasmine S., Rossi, Mariana, Alfè, Dario, Tsatsoulis, Theodoros, Ramberger, Benjamin, Brandenburg, Jan Gerit, Zen, Andrea, Kresse, Georg, Grüneis, Andreas, Tkatchenko, Alexandre, and Michaelides, Angelos. Properties of the water to boron nitride interaction: From zero to two dimensions with benchmark accuracy. United States: N. p., 2017. Web. doi:10.1063/1.4985878.
Al-Hamdani, Yasmine S., Rossi, Mariana, Alfè, Dario, Tsatsoulis, Theodoros, Ramberger, Benjamin, Brandenburg, Jan Gerit, Zen, Andrea, Kresse, Georg, Grüneis, Andreas, Tkatchenko, Alexandre, & Michaelides, Angelos. Properties of the water to boron nitride interaction: From zero to two dimensions with benchmark accuracy. United States. https://doi.org/10.1063/1.4985878
Al-Hamdani, Yasmine S., Rossi, Mariana, Alfè, Dario, Tsatsoulis, Theodoros, Ramberger, Benjamin, Brandenburg, Jan Gerit, Zen, Andrea, Kresse, Georg, Grüneis, Andreas, Tkatchenko, Alexandre, and Michaelides, Angelos. 2017. "Properties of the water to boron nitride interaction: From zero to two dimensions with benchmark accuracy". United States. https://doi.org/10.1063/1.4985878. https://www.osti.gov/servlets/purl/1565595.
@article{osti_1565595,
title = {Properties of the water to boron nitride interaction: From zero to two dimensions with benchmark accuracy},
author = {Al-Hamdani, Yasmine S. and Rossi, Mariana and Alfè, Dario and Tsatsoulis, Theodoros and Ramberger, Benjamin and Brandenburg, Jan Gerit and Zen, Andrea and Kresse, Georg and Grüneis, Andreas and Tkatchenko, Alexandre and Michaelides, Angelos},
abstractNote = {Molecular adsorption on surfaces plays an important part in catalysis, corrosion, desalination, and various other processes that are relevant to industry and in nature. As a complement to experiments, accurate adsorption energies can be obtained using various sophisticated electronic structure methods that can now be applied to periodic systems. The adsorption energy of water on boron nitride substrates, going from zero to 2-dimensional periodicity, is particularly interesting as it calls for an accurate treatment of polarizable electrostatics and dispersion interactions, as well as posing a practical challenge to experiments and electronic structure methods. Here, we present reference adsorption energies, static polarizabilities, and dynamic polarizabilities, for water on BN substrates of varying size and dimension. Adsorption energies are computed with coupled cluster theory, fixed-node quantum Monte Carlo (FNQMC), the random phase approximation, and second order Møller-Plesset theory. These wavefunction based correlated methods are found to agree in molecular as well as periodic systems. The best estimate of the water/h-BN adsorption energy is -107 ± 7 meV from FNQMC. In addition, the water adsorption energy on the BN substrates could be expected to grow monotonically with the size of the substrate due to increased dispersion interactions, but interestingly, this is not the case here. This peculiar finding is explained using the static polarizabilities and molecular dispersion coefficients of the systems, as computed from time-dependent density functional theory (DFT). Dynamic as well as static polarizabilities are found to be highly anisotropic in these systems. Finally, the many-body dispersion method in DFT emerges as a particularly useful estimation of finite size effects for other expensive, many-body wavefunction based methods.},
doi = {10.1063/1.4985878},
url = {https://www.osti.gov/biblio/1565595}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 4,
volume = 147,
place = {United States},
year = {Fri Jul 28 00:00:00 EDT 2017},
month = {Fri Jul 28 00:00:00 EDT 2017}
}

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