Multielectron effects in charge asymmetric molecules induced by asymmetric laser fields.

Using a 45 fs pump pulse at 800 nm, a wave packet is created in a charge asymmetric dissociation channel of iodine, I(2)(2+)→I(2+)+I(0+) (2,0). As the molecule dissociates, a two-color (1ω2ω) probe pulse is used to study the dynamics as a function of internuclear separation R. We find a critical region of R in which there is spatially asymmetric enhanced ionization of the (2,0) channel to a counterintuitive (1,2) channel. In this region the I(0+) is ionized such that one electron is released to the continuum and another is transferred to the I(2+) resulting in I(0+)→I(2+) and I(2+)→I(1+). At larger R, the ionization is consistent with simple one-electron ionization in a double well where I(0+)→I(1+). We find qualitative agreement between simulations and experiment further highlighting the importance of multielectron effects in the strong-field ionization of molecules.