Surface-induced vibrational energy redistribution in methane/surface scattering depends on catalytic activity

Patrick Floß; Christopher S Reilly; Daniel J Auerbach; Rainer D Beck

doi:10.3389/fchem.2023.1238711

Surface-induced vibrational energy redistribution in methane/surface scattering depends on catalytic activity

Front Chem. 2023 Jul 25:11:1238711. doi: 10.3389/fchem.2023.1238711. eCollection 2023.

Authors

Patrick Floß^{1

2}, Christopher S Reilly¹, Daniel J Auerbach^{1

3}, Rainer D Beck^{1

2}

Affiliations

¹ Institute of Chemical Sciences and Engineering (ISIC), École Polytechnique Fédérale de Lausanne (EPFL), Lausanne, Switzerland.
² Max Planck-EPFL Center for Molecular Nanoscience and Technology, Lausanne, Switzerland.
³ Max Planck Institute for Multidisciplinary Sciences, Göttingen, Germany.

Abstract

Recent state-to-state experiments of methane scattering from Ni(111) and graphene-covered Ni(111) combined with quantum mechanical simulations suggest an intriguing correlation between the surface-induced vibrational energy redistribution (SIVR) during the molecule/surface scattering event and the catalytic activity for methane dissociation of the target surface (Werdecker, Phys. Rev. Res., 2020, 2, 043251). Herein, we report new quantum state and angle-resolved measurements for methane scattering from Ni(111) and Au(111) probing the extent of $ν_{3} \to ν_{1}$ antisymmetric-to-symmetric conversion of methane stretching motion for two surfaces with different catalytic activities. Consistent with the expectations, the extent of SIVR occurring on the more catalytically active Ni(111) surface, as measured by the $ν_{1} : ν_{3}$ scattered population ratio, is found to be several times stronger than that on the more inert Au(111) surface. We also present additional insights on the rovibrational scattering dynamics contained in the angle- and state-resolved data. The results together highlight the power of state-resolved scattering measurements as a tool for investigating methane-surface interactions.

Keywords: angular distributions; bolometer infrared laser tagging; heterogeneous catalysis; methane dissociation; optothermal spectroscopy; state-to-state scattering; surface-induced vibrational energy redistribution.