Generation of Sub-nanosecond H Atom Pulses for Scattering from Single-Crystal Epitaxial Graphene.

Pulsed molecular beams allow high-density gas samples to be cooled to low internal temperatures and to produce narrow speed distributions. They are particularly useful in combination with pulsed-laser-based detection schemes and have also been used as pump pulses in pump-probe experiments with neutral matter. The mechanical response of pulsed valves and chopper wheels limits the duration of these pulses typically to about 10-100 μs. Bunch compression photolysis has been proposed as a means to produce atomic pulses shorter than 1 ns─an experimental capability that would allow new measurements to be made on chemical systems. This technique employs a spatially chirped femtosecond duration photolysis pulse that produced an ensemble of H atom photoproducts that rebunches into a short pulse downstream. To date, this technique could not produce strong enough beams to allow new experiments to be carried out. In this paper, we report production of pulsed H atom beams consistent with a 700 ps pulse duration and with sufficient intensity to carry out differentially resolved inelastic H scattering experiments from a graphene surface. We observe surprisingly narrow angular distributions for H atoms incident normal to the surface. At low incidence energies quasi-elastic scattering dominates, and at high incidence energy we observe a strongly inelastic scattering channel. These results provide the basis for future experiments where the H atoms synchronously collide with a pulsed-laser-excited surface.