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Quaranta V, Hellström M, Behler J, et al. Maximally resolved anharmonic OH vibrational spectrum of the water/ZnO(101¯0) interface from a high-dimensional neural network potential. J Chem Phys. 2018;148(24):241720doi: 10.1063/1.5012980.
Quaranta, V., Hellström, M., Behler, J., Kullgren, J., Mitev, P. D., & Hermansson, K. (2018). Maximally resolved anharmonic OH vibrational spectrum of the water/ZnO(101¯0) interface from a high-dimensional neural network potential. The Journal of chemical physics, 148(24), 241720. https://doi.org/10.1063/1.5012980
Quaranta, Vanessa, et al. "Maximally resolved anharmonic OH vibrational spectrum of the water/ZnO(101¯0) interface from a high-dimensional neural network potential." The Journal of chemical physics vol. 148,24 (2018): 241720. doi: https://doi.org/10.1063/1.5012980
Quaranta V, Hellström M, Behler J, Kullgren J, Mitev PD, Hermansson K. Maximally resolved anharmonic OH vibrational spectrum of the water/ZnO(101¯0) interface from a high-dimensional neural network potential. J Chem Phys. 2018 Jun 28;148(24):241720. doi: 10.1063/1.5012980. PMID: 29960340.
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J Chem Phys. 2018 Jun 28;148(24):241720. doi: 10.1063/1.5012980.

Maximally resolved anharmonic OH vibrational spectrum of the water/ZnO(101¯0) interface from a high-dimensional neural network potential.

The Journal of chemical physics

Vanessa Quaranta, Matti Hellström, Jörg Behler, Jolla Kullgren, Pavlin D Mitev, Kersti Hermansson

Affiliations

  1. Lehrstuhl für Theoretische Chemie, Ruhr-Universität Bochum, D-44780 Bochum, Germany.
  2. Department of Chemistry-Ångström Laboratory, Uppsala University, P.O. Box 538, SE-75121 Uppsala, Sweden.

PMID: 29960340 DOI: 10.1063/1.5012980

Abstract

Unraveling the atomistic details of solid/liquid interfaces, e.g., by means of vibrational spectroscopy, is of vital importance in numerous applications, from electrochemistry to heterogeneous catalysis. Water-oxide interfaces represent a formidable challenge because a large variety of molecular and dissociated water species are present at the surface. Here, we present a comprehensive theoretical analysis of the anharmonic OH stretching vibrations at the water/ZnO(101¯0) interface as a prototypical case. Molecular dynamics simulations employing a reactive high-dimensional neural network potential based on density functional theory calculations have been used to sample the interfacial structures. In the second step, one-dimensional potential energy curves have been generated for a large number of configurations to solve the nuclear Schrödinger equation. We find that (i) the ZnO surface gives rise to OH frequency shifts up to a distance of about 4 Å from the surface; (ii) the spectrum contains a number of overlapping signals arising from different chemical species, with the frequencies decreasing in the order ν(adsorbed hydroxide) > ν(non-adsorbed water) > ν(surface hydroxide) > ν(adsorbed water); (iii) stretching frequencies are strongly influenced by the hydrogen bond pattern of these interfacial species. Finally, we have been able to identify substantial correlations between the stretching frequencies and hydrogen bond lengths for all species.

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