Echo-assisted impulsive alignment of room-temperature acetone molecules

2021

International audience; We experimentally and theoretically investigate the field-free alignment of the asymmetric-top acetone molecule. Our study shows that the production of postpulse aligned molecules in a dense sample (0.05-0.2 bar) of room-temperature acetone using a single-pulse excitation can be significantly improved by rotational alignment echoes induced in a two-pulse excitation scheme. We report the observation of fractional echoes that can be used to reveal the nonlinearity of the molecular system. In a proof-of-principle experiment, a pre-aligned sample of acetone is also used for third-harmonic generation. The analysis of the experimental data with numerical simulations based …