Nalazite se na CroRIS probnoj okolini. Ovdje evidentirani podaci neće biti pohranjeni u Informacijskom sustavu znanosti RH. Ako je ovo greška, CroRIS produkcijskoj okolini moguće je pristupi putem poveznice www.croris.hr
izvor podataka: crosbi

Vibrational response and motion of carbon monoxide on Cu(100) driven by femtosecond laser pulses: Molecular dynamics with electronic friction (CROSBI ID 273390)

Prilog u časopisu | izvorni znanstveni rad | međunarodna recenzija

Scholz, Robert ; Lindner, Steven ; Lončarić, Ivor ; Tremblay, Jean Christophe ; Juaristi, J. I. ; Alducin, M. ; Saalfrank, Peter Vibrational response and motion of carbon monoxide on Cu(100) driven by femtosecond laser pulses: Molecular dynamics with electronic friction // Physical review. B, 100 (2019), 24; 245431, 20. doi: 10.1103/physrevb.100.245431

Podaci o odgovornosti

Scholz, Robert ; Lindner, Steven ; Lončarić, Ivor ; Tremblay, Jean Christophe ; Juaristi, J. I. ; Alducin, M. ; Saalfrank, Peter

engleski

Vibrational response and motion of carbon monoxide on Cu(100) driven by femtosecond laser pulses: Molecular dynamics with electronic friction

Carbon monoxide on copper surfaces continues to be a fascinating, rich microlab for many questions evolving in surface science. Recently, hot-electron mediated, femtosecond-laser pulse induced dynamics of CO molecules on Cu(100) were the focus of experiments [Inoue et al., Phys. Rev. Lett. 117, 186101 (2016)] and theory [Novko et al., Phys. Rev. Lett. 122, 016806 (2019)], unraveling details of the vibrational nonequilibrium dynamics on ultrashort (subpicoseconds) timescales. In the present work, full-dimensional time-resolved hot-electron driven dynamics are studied by molecular dynamics with electronic friction (MDEF). Dissipation is included by a friction term in a Langevin equation which describes the coupling of molecular degrees of freedom to electron-hole pairs in the copper surface, calculated from gradient-corrected density functional theory (DFT) via a local density friction approximation (LDFA). Relaxation due to surface phonons is included by a generalized Langevin oscillator model. The hot-electron induced excitation is described via a time-dependent electronic temperature, the latter derived from an improved two-temperature model. Our parameter-free simulations on a precomputed potential energy surface allow for excellent statistics, and the observed trends are confirmed by on-the-fly ab initio molecular dynamics with electronic friction (AIMDEF) calculations. By computing time-resolved frequency maps for selected molecular vibrations, instantaneous frequencies, probability distributions, and correlation functions, we gain microscopic insight into hot- electron driven dynamics and we can relate the time evolution of vibrational internal CO stretch-mode frequencies to measured data, notably an observed redshift. Quantitatively, the latter is found to be larger in MDEF than in experiment and possible reasons are discussed for this observation. In our model, in addition we observe the excitation and time evolution of large-amplitude low-frequency modes, lateral CO surface diffusion, and molecular desorption. Effects of surface atom motion and of the laser fluence are also discussed.

molecular dynamics

nije evidentirano

nije evidentirano

nije evidentirano

nije evidentirano

nije evidentirano

nije evidentirano

Podaci o izdanju

100 (24)

2019.

245431

20

objavljeno

2469-9950

2469-9969

10.1103/physrevb.100.245431

Povezanost rada

Fizika

Poveznice
Indeksiranost