AUTHOR=Floß Patrick , Reilly Christopher S. , Auerbach Daniel J. , Beck Rainer D. 

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

JOURNAL=Frontiers in Chemistry

VOLUME=11

YEAR=2023

URL=https://www.frontiersin.org/journals/chemistry/articles/10.3389/fchem.2023.1238711

DOI=10.3389/fchem.2023.1238711

ISSN=2296-2646

ABSTRACT=<p>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 <inline-formula id="inf1"><mml:math id="m1" xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:msub><mml:mi>ν</mml:mi><mml:mn>3</mml:mn></mml:msub><mml:mo>→</mml:mo><mml:msub><mml:mi>ν</mml:mi><mml:mn>1</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> 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 <inline-formula id="inf2"><mml:math id="m2" xmlns:mml="http://www.w3.org/1998/Math/MathML"><mml:mrow><mml:msub><mml:mi>ν</mml:mi><mml:mn>1</mml:mn></mml:msub><mml:mo>:</mml:mo><mml:msub><mml:mi>ν</mml:mi><mml:mn>3</mml:mn></mml:msub></mml:mrow></mml:math></inline-formula> 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.</p>