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Título: | Ultrafast transient dynamics of adsorbates on surfaces deciphered: The case of CO on Cu(100) |
Autor: | Novko, Dino; Tremblay, J. C.; Alducin Ochoa, Maite CSIC ORCID ; Juaristi Oliden, Joseba Iñaki CSIC ORCID | Fecha de publicación: | 2019 | Editor: | American Physical Society | Citación: | Physical Review Letters 122(3): 016806 (2019) | Resumen: | Time-resolved vibrational spectroscopy constitutes an invaluable experimental tool for monitoring hotcarrier-induced surface reactions. However, the absence of a full understanding of the precise microscopic mechanisms causing the transient spectral changes has limited its applicability. Here we introduce a robust first-principles theoretical framework that successfully explains both the nonthermal frequency and linewidth changes of the CO internal stretch mode on Cu(100) induced by femtosecond laser pulses. Two distinct processes engender the changes: electron-hole pair excitations underlie the nonthermal frequency shifts, while electron-mediated vibrational mode coupling gives rise to linewidth changes. Furthermore, the origin and precise sequence of coupling events are finally identified. | Versión del editor: | https://doi.org/10.1103/PhysRevLett.122.016806 | URI: | http://hdl.handle.net/10261/178626 | ISSN: | 0031-9007 10.1103/PhysRevLett.122.016806 |
E-ISSN: | 1079-7114 |
Aparece en las colecciones: | (CFM) Artículos |
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