Two distinctive energy migration pathways of monolayer molecules on metal nanoparticle surfaces

Jiebo Li, Huifeng Qian, Hailong Chen, Zhun Zhao, Kaijun Yuan, Guangxu Chen, Andrea Miranda, Xunmin Guo, Yajing Chen, Nanfeng Zheng, Michael S. Wong and Junrong Zheng ()
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Jiebo Li: College of Chemistry and Molecular Engineering, Beijing National Laboratory for Molecular Sciences, Peking University
Huifeng Qian: Rice University, 6100 Main Street, Houston, Texas 77005, USA
Hailong Chen: Rice University, 6100 Main Street, Houston, Texas 77005, USA
Zhun Zhao: Rice University, 6100 Main Street, Houston, Texas 77005, USA
Kaijun Yuan: State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of the Chemical Physics, Chinese Academy of Sciences
Guangxu Chen: College of Chemistry and Chemical Engineering, Xiamen University
Andrea Miranda: Rice University, 6100 Main Street, Houston, Texas 77005, USA
Xunmin Guo: Rice University, 6100 Main Street, Houston, Texas 77005, USA
Yajing Chen: State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of the Chemical Physics, Chinese Academy of Sciences
Nanfeng Zheng: College of Chemistry and Chemical Engineering, Xiamen University
Michael S. Wong: Rice University, 6100 Main Street, Houston, Texas 77005, USA
Junrong Zheng: College of Chemistry and Molecular Engineering, Beijing National Laboratory for Molecular Sciences, Peking University

Nature Communications, 2016, vol. 7, issue 1, 1-8

Abstract: Abstract Energy migrations at metal nanomaterial surfaces are fundamentally important to heterogeneous reactions. Here we report two distinctive energy migration pathways of monolayer adsorbate molecules on differently sized metal nanoparticle surfaces investigated with ultrafast vibrational spectroscopy. On a 5 nm platinum particle, within a few picoseconds the vibrational energy of a carbon monoxide adsorbate rapidly dissipates into the particle through electron/hole pair excitations, generating heat that quickly migrates on surface. In contrast, the lack of vibration-electron coupling on approximately 1 nm particles results in vibrational energy migration among adsorbates that occurs on a twenty times slower timescale. Further investigations reveal that the rapid carbon monoxide energy relaxation is also affected by the adsorption sites and the nature of the metal but to a lesser extent. These findings reflect the dependence of electron/vibration coupling on the metallic nature, size and surface site of nanoparticles and its significance in mediating energy relaxations and migrations on nanoparticle surfaces.

Date: 2016
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DOI: 10.1038/ncomms10749

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