Full quantum dynamics study for H atom scattering from graphene

• Verfasst von: Shi, Lei [VerfasserIn]
• Verfasst von: Schröder, Markus [VerfasserIn]
• Verfasst von: Meyer, Hans-Dieter [VerfasserIn]
• Verfasst von: Peláez, Daniel [VerfasserIn]
• Verfasst von: Wodtke, Alec Michael [VerfasserIn]
• Verfasst von: Golibrzuch, Kai [VerfasserIn]
• Verfasst von: Schönemann, Anna-Maria [VerfasserIn]
• Verfasst von: Kandratsenka, Alexander [VerfasserIn]
• Verfasst von: Gatti, Fabien [VerfasserIn]
• Titel: Full quantum dynamics study for H atom scattering from graphene
• Verf.angabe: Lei Shi, Markus Schröder, Hans-Dieter Meyer, Daniel Peláez, Alec M. Wodtke, Kai Golibrzuch, Anna-Maria Schönemann, Alexander Kandratsenka and Fabien Gatti
• E-Jahr: 2025
• Jahr: January 14, 2025
• Umfang: 12 S.
• Illustrationen: Illustrationen
• Fussnoten: Gesehen am 23.05.2025
• Titel Quelle: Enthalten in: The journal of physical chemistry. A, Molecules, clusters, and aerosols
• Ort Quelle: Washington, DC : American Chemical Society, 1997
• Jahr Quelle: 2025
• Band/Heft Quelle: 129(2025), 7, Seite 1896-1907
• ISSN Quelle: 1520-5215
• DOI: doi:10.1021/acs.jpca.4c06712
• Datenträger: Online-Ressource
• Sprache: eng
• K10plus-PPN: 1926406060

Abstract

This study deals with the understanding of hydrogen atom scattering from graphene, a process critical for exploring C-H bond formation and energy transfer during atom surface collision. In our previous work [Shi, L.; J. Chem. Phys. 2023, 159, 194102], starting from a cell with 24 carbon atoms treated periodically, we have achieved quantum dynamics (QD) simulations with a reduced-dimensional model (15D) and a simulation in full dimensionality (75D). In the former work, the H atom attacked the top of a single C atom, enabling a comparison of QD simulation results to classical molecular dynamics (cMD). Our approach required the use of sophisticated techniques such as Monte Carlo canonical polyadic decomposition (MCCPD) and multilayer multiconfiguration time-dependent Hartree (ML-MCTDH), as well as further development of quantum flux calculations. We could benchmark our calculations by comparison to cMD calculations. We now refined our method to better mimic experimental conditions. Specifically, rather than sending the H atom to a specific position on the surface, we employed a plane wave for the H atom in directions parallel to the surface. Key findings for these new simulations include the identification of discrepancies between classical molecular dynamics (cMD) simulations and experiments, which are attributed to both the potential energy surface (PES) and quantum effects. Additionally, this study sheds light on the role of classical collective normal modes during collisions, providing insights into energy transfer processes. The results validate the robustness of our simulation methodologies and highlight the importance of considering quantum mechanical effects in the study of hydrogen-graphene interactions.