Jiang, Hongyan and Tao, Xuecheng and Kammler, Marvin and Ding, Feizhi and Wodtke, Alec M. and Kandratsenka, Alexander and Miller, Thomas F., III and Bünermann, Oliver (2021) Small Nuclear Quantum Effects in Scattering of H and D from Graphene. Journal of Physical Chemistry Letters, 12 (7). pp. 1991-1996. ISSN 1948-7185. doi:10.1021/acs.jpclett.0c02933. https://resolver.caltech.edu/CaltechAUTHORS:20210218-150439555
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Abstract
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.
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| Additional Information: | © 2021 American Chemical Society. Received: September 24, 2020; Accepted: February 10, 2021; Published: February 17, 2021. X.T. acknowledges support from the Department of Dynamics at Surfaces at the MPI for Biophysical Chemistry and ICASEC at the University of Goettingen during the visit. H.J., O.B., and A.M.W. acknowledge support the from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation, 217133147/SFB 1073, project A04) and financial support from the Ministerium für Wissenschaft und Kultur (MWK) Niedersachsen and the Volkswagenstiftung under grant no. INST 186/902-1 to build the experimental apparatus. A.M.W., M.K., and A.K. also acknowledge the Max Planck Society for the Advancement of Science. F.D. and T.F.M. acknowledge that this material is based on work performed by the Joint Center for Artificial Photosynthesis, a U.S. Department of Energy (DOE) Energy Innovation Hub, supported through the Office of Science of the DOE under award DE-SC0004993; X.T. and T.F.M. acknowledge support from the DOE (DE-SC0019390) and also thank the National Energy Research Scientific Computing Center for the computational resources. We thank Dan Auerbach and Dirk Schwarzer for helpful discussions. Author Contributions: H.J. and X.T. contributed equally to this work. The authors declare the following competing financial interest(s): Calculations performed in this work use the Entos Qcore simulation software, and Thomas Miller is a co-founder Entos, Inc. | ||||||||||||||||
| Group: | JCAP | ||||||||||||||||
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| Issue or Number: | 7 | ||||||||||||||||
| DOI: | 10.1021/acs.jpclett.0c02933 | ||||||||||||||||
| Record Number: | CaltechAUTHORS:20210218-150439555 | ||||||||||||||||
| Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20210218-150439555 | ||||||||||||||||
| Official Citation: | Small Nuclear Quantum Effects in Scattering of H and D from Graphene. Hongyan Jiang, Xuecheng Tao, Marvin Kammler, Feizhi Ding, Alec M. Wodtke, Alexander Kandratsenka, Thomas F. Miller, and Oliver Bünermann. The Journal of Physical Chemistry Letters 0, 12; DOI: 10.1021/acs.jpclett.0c02933 | ||||||||||||||||
| Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | ||||||||||||||||
| ID Code: | 108107 | ||||||||||||||||
| Collection: | CaltechAUTHORS | ||||||||||||||||
| Deposited By: | Tony Diaz | ||||||||||||||||
| Deposited On: | 18 Feb 2021 23:18 | ||||||||||||||||
| Last Modified: | 16 Nov 2021 19:09 |
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