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

[Image: see text] 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.