Small Nuclear Quantum Effects in Scattering of H and D from Graphene

We study nuclear quantum effects in H/D sticking to graphene, comparing scattering experiments at near-zero coverage with classical, quantized, and transition-state calculations. The experiment shows H/D sticking probabilities that are indistinguishable from one another and markedly smaller than tho...

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Bibliographic Details
Published in:The journal of physical chemistry letters 2021-02, Vol.12 (7), p.1991-1996
Main Authors: Jiang, Hongyan, Tao, Xuecheng, Kammler, Marvin, Ding, Feizhi, Wodtke, Alec M, Kandratsenka, Alexander, Miller, Thomas F, Bünermann, Oliver
Format: Article
Language:English
Subjects:
Chemistry
Materials Science
Physical Insights into Chemistry, Catalysis, and Interfaces
Physics
Science & Technology - Other Topics
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Summary:We study nuclear quantum effects in H/D sticking to graphene, comparing scattering experiments at near-zero coverage with classical, quantized, and transition-state calculations. The experiment shows H/D sticking probabilities that are indistinguishable from one another and markedly smaller than those expected from a consideration of zero-point energy shifts of the chemisorption transition state. Inclusion of dynamical effects and vibrational anharmonicity via ring-polymer molecular dynamics (RPMD) yields results that are in good agreement with the experimental results. RPMD also reveals that nuclear quantum effects, while modest, arise primarily from carbon and not from H/D motion, confirming the importance of a C atom rehybridization mechanism associated with H/D sticking on graphene.
ISSN:1948-7185
1948-7185
DOI:10.1021/acs.jpclett.0c02933