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Valence molecular orbitals play a crucial role in chemical reactions. Here wereveal that an intense laser field deforms an inner valence orbital (10a') inthe ethanol molecule. We measure the recoil-frame photoelectron angulardistribution (RFPAD), which corresponds to the orientation dependence of theionization probability of the orbital, using photoelectron-photoion coincidencemomentum imaging with a circularly polarized laser pulse. Ab initio simulationsshow that the orbital deformation depends strongly on the laser fielddirection, and that the measured RFPAD cannot be reproduced without taking theorbital deformation into account. Our findings suggest that the laser-inducedorbital deformation occurs prior to electron emission on a sub-optical-cycletime scale.

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