Femtosecond laser activation of surface reactions

Abstract:

Laser induced formation of CO2 and desorption of O 2 are initiated with femtosecond and picosecond laser excitation of a Pt(111) surface prepared with coadsorbed CO and O2 at 90 K. The nonlinear fluence dependent reaction yields were measured for 267, 400, and 800 nm wavelengths, and for pulse durations from 80 fs to 3.6 ps. Two- pulse correlation experiments measuring total O2 desorption yield versus time delay between 80 fs pulses show a 0.9 ps HWHM central peak and a slower 0.1 ns time-scale. At 267 nm the relative yields of O2 and CO2 are found to depend on fluence. Comparison of results at different wavelengths and pulsewidths shows that nonthermalized surface electrons play a role in the laser-induced surface chemistry.