Spatial and temporal control of populations, branching ratios, and electronic coherences in LiH by a single one-cycle infrared pulse

Dynamical computations demonstrate considerable selectivity over the fragmentation channels of the LiH molecule via the polarization and the carrier envelope phase (CEP) of a single ultrashort one-cycle strong IR pulse. For aligned molecules, control of the CEP allows building nonstationary coherent electronic wave packets of contrasting ionic character, either Liδ+Hδ- or Liδ-Hδ+. The complementary coherences are maintained all the way to dissociation. The direction of the electric field at its maximum points either towards the Li or towards the H atom, which selectively steers the nuclear dynamics to specific dissociation products.