Naslov
Ultrafast Transient Dynamics of Adsorbates on Surfaces Deciphered: The Case of CO on Cu(100)

Autori
Novko, D. ; Tremblay, J. C. ; Alducin, M. ; Juaristi, J. I.

Izvornik
Physical Review Letters (0031-9007) 122 (2019), 1; 016806, 5

Vrsta, podvrsta i kategorija rada
Radovi u časopisima, članak, znanstveni

Ključne riječi
electron-phonon coupling, ultrafast vibrational relaxation

Sažetak
Time-resolved vibrational spectroscopy constitutes an invaluable experimental tool for monitoring hot-carrier-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.

Izvorni jezik
Engleski

Znanstvena područja
Fizika

POVEZANOST RADA