Electron-Mediated Phonon-Phonon Coupling Drives the Vibrational Relaxation of CO on Cu(100)

Physical Review Letters
D NovkoJ I Juaristi

Abstract

We bring forth a consistent theory for the electron-mediated vibrational intermode coupling that clarifies the microscopic mechanism behind the vibrational relaxation of adsorbates on metal surfaces. Our analysis points out the inability of state-of-the-art nonadiabatic theories to quantitatively reproduce the experimental linewidth of the CO internal stretch mode on Cu(100) and it emphasizes the crucial role of the electron-mediated phonon-phonon coupling in this regard. The results demonstrate a strong electron-mediated coupling between the internal stretch and low-energy CO modes, but also a significant role of surface motion. Our nonadiabatic theory is also able to explain the temperature dependence of the internal stretch phonon linewidth, thus far considered a sign of the direct anharmonic coupling.

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Citations

Mar 12, 2020·Physical Chemistry Chemical Physics : PCCP·Tobias SerwatkaJean Christophe Tremblay
Aug 10, 2018·Physical Chemistry Chemical Physics : PCCP·Oihana GalparsoroPascal Larregaray
May 10, 2019·The Journal of Chemical Physics·Natalia García Rey, Heike Arnolds
Jan 11, 2020·Physical Review Letters·Maite AlducinJ Iñaki Juaristi
Feb 20, 2019·The Journal of Physical Chemistry Letters·Ivor LončarićD Novko
May 16, 2019·The Journal of Physical Chemistry Letters·Paul SpieringJörg Meyer

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