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

被引：30

作者：

Novko, D. ^{[1
,2
]}

Tremblay, J. C. ^{[3
]}

Alducin, M. ^{[2
,4
]}

Juaristi, J. I. ^{[2
,4
,5
]}

机构：

[1] Inst Phys, Ctr Excellence Adv Mat & Sensing Devices, Bijenicka 46, Zagreb 10000, Croatia

[2] Donostia Int Phys Ctr DIPC, Paseo Manuel Lardizabal 4, Donostia San Sebastian 20018, Spain

[3] Free Univ Berlin, Inst Chem & Biochem, Takustr 3, D-14195 Berlin, Germany

[4] Ctr Fis Mat CSIC UPV EHU, Paseo Manuel Lardizabal 5, Donostia San Sebastian 20018, Spain

[5] Fac Quim UPV EHU, Dept Fis Mat, Apartado 1072, Donostia San Sebastian 20080, Spain

来源：

PHYSICAL REVIEW LETTERS | 2019年 / 122卷 / 01期

关键词：

REAL-TIME OBSERVATION; LASER-INDUCED DESORPTION; ELECTRON; MOTION; PHONON; SPECTROSCOPY; RELAXATION; EXCITATION; VIBRATIONS; RU(001);

D O I：

10.1103/PhysRevLett.122.016806

中图分类号：

O4 [物理学];

学科分类号：

0702 ;

摘要：

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.

引用

页数：5

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