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  Quantum Nuclei at Weakly Bonded Interfaces: The Case of Cyclohexane on Rh(111)

Fidanyan, K., Hamada, I., & Rossi, M. (2021). Quantum Nuclei at Weakly Bonded Interfaces: The Case of Cyclohexane on Rh(111). Advanced Theory and Simulations, 2000241. doi:10.1002/adts.202000241.

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Fidanyan, Karen1, 2, Author              
Hamada, Ikutaro3, Author
Rossi, Mariana1, 2, Author              
Affiliations:
1Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, Hamburg, 22761 Germany, ou_persistent22              
2NOMAD, Fritz Haber Institute, Max Planck Society, ou_3253022              
3Department of Precision Engineering, Graduate School of Engineering, Osaka University, 2‐1 Yamadaoka, Suita, Osaka, 565‐0871 Japan, ou_persistent22              

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 Abstract: The electronic properties of interfaces can depend on their isotopic constitution. One known case is that of cyclohexane physisorbed on Rh(111), in which isotope effects have been measured on the work function change and desorption energies. These effects can only be captured by calculations including nuclear quantum effects (NQE). In this paper, this interface is addressed employing dispersion‐inclusive density‐functional theory coupled to a quasi‐harmonic (QH) approximation for NQE, as well as to fully anharmonic ab initio path integral molecular dynamics (PIMD). The QH approximation is able to capture that deuterated cyclohexane has a smaller adsorption energy and lies about 0.01 Å farther from the Rh(111) surface than its isotopologue, which can be correlated to the isotope effect in the work function change. An investigation of the validity of the QH approximation relying on PIMD simulations, leads to the conclusion that although this interface is highly impacted by anharmonic quantum fluctuations in the molecular layer and at bonding sites, these anharmonic contributions play a minor role when analyzing isotope effects at low temperatures. Nevertheless, anharmonic quantum fluctuations cause an increase in the distance between the molecular layer and Rh(111), a consequent smaller overall work function change, and intricate changes in orbital hybridization.

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Language(s): eng - English
 Dates: 2020-12-222020-09-302021-01-14
 Publication Status: Published online
 Pages: 10
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/adts.202000241
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Title: Advanced Theory and Simulations
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH Verlag
Pages: 10 Volume / Issue: - Sequence Number: 2000241 Start / End Page: - Identifier: ISSN: 2513-0390
CoNE: https://pure.mpg.de/cone/journals/resource/2513-0390