Deformation of an inner valence molecular orbital in ethanol by an intense laser field

Valence molecular orbitals play a crucial role in chemical reactions. Here, we reveal that an intense laser field deforms an inner valence orbital (10a′) in the ethanol molecule. We measure the recoil-frame photoelectron angular distribution (RFPAD), which corresponds to the orientation dependence of the ionization probability of the orbital, using photoelectron-photoion coincidence momentum imaging with a circularly polarized laser pulse. Ab initio simulations show that the orbital deformation depends strongly on the laser field direction and that the measured RFPAD cannot be reproduced without taking the orbital deformation into account. Our findings suggest that the laser-induced orbital deformation occurs before electron emission on a suboptical cycle time scale.

Asymmetry flip in photoelectron angular distribution of rare gas atoms in intense circularly-polarized few-cycle laser fields

An analytical formula representing the photoelectron kinetic energy at which the ejection direction of photoelectrons generated by an intense circularly-polarized few-cycle laser pulse flips was derived and was used for determining the laser pulse duration.