Article (Scientific journals)
Properties of the water to boron nitride interaction: from zero to two dimensions with benchmark accuracy
Al-Hamdani, Yasmine; Rossi, Mariana; Alfè, Dario et al.
2017In Journal of Chemical Physics, 147, p. 044710
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Abstract :
[en] 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. In addition, 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.
Disciplines :
Physics
Author, co-author :
Al-Hamdani, Yasmine ;  University of Luxembourg > Faculty of Science, Technology and Communication (FSTC) > Physics and Materials Science Research Unit
Rossi, Mariana
Alfè, Dario
Tsatsoulis, Theodoros
Ramberger, Benjamin
Brandenburg, Jan Gerit
Zen, Andrea
Kresse
Grüneis, Andreas
Tkatchenko, Alexandre ;  University of Luxembourg > Faculty of Science, Technology and Communication (FSTC) > Physics and Materials Science Research Unit
Michaelides, Angelos
External co-authors :
yes
Language :
English
Title :
Properties of the water to boron nitride interaction: from zero to two dimensions with benchmark accuracy
Publication date :
July 2017
Journal title :
Journal of Chemical Physics
ISSN :
1089-7690
Publisher :
American Institute of Physics, New York, United States - New York
Volume :
147
Pages :
044710
Peer reviewed :
Peer Reviewed verified by ORBi
Focus Area :
Physics and Materials Science
European Projects :
FP7 - 616121 - HETEROICE - Towards a molecular-level understanding of heterogeneous ice nucleation
Funders :
CE - Commission Européenne [BE]
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since 09 August 2017

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