Sub-Femtosecond Stark Control of Molecular Photoexcitation with Near Single-Cycle Pulses.

Electric fields can tailor molecular potential energy surfaces by interaction with the electronic state-dependent molecular dipole moment. Recent developments in optics have enabled the creation of ultrashort few-cycle optical pulses with precise control of the carrier envelope phase (CEP) that determines the offset of the maxima in the field and the pulse envelope. This opens news ways of controlling ultrafast molecular dynamics by exploiting the CEP. In this work, we show that the photoabsorption efficiency of oriented HCSO (sulfine) can be controlled by tuning the CEP. We further show that this control emanates from a resonance condition related to Stark shifting of the electronic energy levels.