Generation of ultra-short hydrogen atom pulses by bunch-compression photolysis

Ultra-short light pulses enable many time-resolved studies in chemistry, especially when used in pump-probe experiments. However, most chemical events are not initiated by light, but rather by collisions. Time-resolved collisional experiments require ultra-short pulses of atoms and molecules--sadly, methods for producing such pulses are so far unknown. Here we introduce bunch-compression photolysis, an approach to forming ultra-short and highly intense pulses of neutral atoms. We demonstrate H-atom pulses of 1.2±0.3 ns duration, far shorter than any previously reported. Owing to its extraordinarily simple physical principles, we can accurately model the method--the model shows H-atom pulses as short as 110-ps are achievable. Importantly, due to the bunch-compression, large (mm(3)) photolysis volumes are possible, a key advantage for pulse intensity. This technique overcomes the most challenging barrier to a new class of experiments on time-resolved collisions involving atoms and molecules.