TY  - JOUR
A1  - Füchsel, Gernot
A1  - Klamroth, Tillmann
A1  - Monturet, Serge
A1  - Saalfrank, Peter
T1  - Dissipative dynamics within the electronic friction approach the femtosecond laser desorption of H-2/D-2 from Ru(0001)
T2  - Physical chemistry, chemical physics : a journal of European Chemical Societies
N2  - An electronic friction approach based on Langevin dynamics is used to describe the multidimensional (six-dimensional) dynamics of femtosecond laser induced desorption of H-2 and D-2 from a H(D)-covered Ru(0001) surface. The paper extends previous reduced-dimensional models, using a similar approach. In the present treatment forces and frictional coefficients are calculated from periodic density functional theory (DFT) and essentially parameter-free, while the action of femtosecond laser pulses on the metal surface is treated by using the two-temperature model. Our calculations shed light on the performance and validity of various adiabatic, non-adiabatic, and Arrhenius/Kramers type kinetic models to describe hot-electron mediated photoreactions at metal surfaces. The multidimensional frictional dynamics are able to reproduce and explain known experimental facts, such as strong isotope effects, scaling of properties with laser fluence, and non-equipartitioning of vibrational, rotational, and translational energies of desorbing species. Further, detailed predictions regarding translations are made, and the question for the controllability of photoreactions at surfaces with the help of vibrational preexcitation is addressed.
Y1  - 2011
UR  - https://publishup.uni-potsdam.de/frontdoor/index/index/docId/37227
SN  - 1463-9076
VL  - 13
IS  - 19
SP  - 8659
EP  - 8670
PB  - Royal Society of Chemistry
CY  - Cambridge
ER  -