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  4. Decisive role of nuclear quantum effects on surface mediated water dissociation at finite temperature
 
research article

Decisive role of nuclear quantum effects on surface mediated water dissociation at finite temperature

Litman, Yair
•
Donadio, Davide
•
Ceriotti, Michele  
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2018
The Journal of Chemical Physics

Water molecules adsorbed on inorganic substrates play an important role in several technological applications. In the presence of light atoms in adsorbates, nuclear quantum effects (NQEs) influence the structural stability and the dynamical properties of these systems. In this work, we explore the impact of NQEs on the dissociation of water wires on stepped Pt(221) surfaces. By performing ab initio molecular dynamics simulations with van der Waals corrected density functional theory, we note that several competing minima for both intact and dissociated structures are accessible at finite temperatures, making it important to assess whether harmonic estimates of the quantum free energy are sufficient to determine the relative stability of the different states. We thus perform ab initio path integral molecular dynamics (PIMD) in order to calculate these contributions taking into account the conformational entropy and anharmonicities at finite temperatures. We propose that when adsorption is weak and NQEs on the substrate are negligible, PIMD simulations can be performed through a simple partition of the system, resulting in considerable computational savings. We then calculate the full contribution of NQEs to the free energies, including also anharmonic terms. We find that they result in an increase of up to 20% of the quantum contribution to the dissociation free energy compared with the harmonic estimates. We also find that the dissociation process has a negligible contribution from tunneling but is dominated by zero point energies, which can enhance the rate of dissociation by three orders of magnitude. Finally we highlight how both temperature and NQEs indirectly impact dipoles and the redistribution of electron density, causing work function changes of up to 0.4 eV with respect to static estimates. This quantitative determination of the change in the work function provides a possible approach to determine experimentally the most stable configurations of water oligomers on the stepped surfaces.

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Type
research article
DOI
10.1063/1.5002537
Web of Science ID

WOS:000427517200024

Author(s)
Litman, Yair
Donadio, Davide
Ceriotti, Michele  
Rossi, Mariana
Date Issued

2018

Published in
The Journal of Chemical Physics
Volume

148

Issue

10

Article Number

102320

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
COSMO  
FunderGrant Number

H2020

ERC 677013-HBMAP

FNS

SNSF 200021-159896 NQE

Available on Infoscience
November 19, 2019
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/163192
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