Reference : Properties of the water to boron nitride interaction: from zero to two dimensions wit...
Scientific journals : Article
Physical, chemical, mathematical & earth Sciences : Physics
Physics and Materials Science
http://hdl.handle.net/10993/31866
Properties of the water to boron nitride interaction: from zero to two dimensions with benchmark accuracy
English
Al-Hamdani, Yasmine mailto [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 mailto [University of Luxembourg > Faculty of Science, Technology and Communication (FSTC) > Physics and Materials Science Research Unit >]
Michaelides, Angelos []
Jul-2017
Journal of Chemical Physics
American Institute of Physics
147
044710
Yes (verified by ORBilu)
International
0021-9606
1089-7690
New York
NY
[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.
Researchers ; Students
http://hdl.handle.net/10993/31866
10.1063/1.4985878
FP7 ; 616121 - HETEROICE - Towards a molecular-level understanding of heterogeneous ice nucleation

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