Robust Ultrafast Currents in Molecular Wires through Stark Shifts

A novel way to induce ultrafast currents in molecular wires using two incident laser frequencies, omega and 2omega, is demonstrated. The mechanism relies on Stark shifts, instead of near-resonance photon absorption, to transfer population to the excited states and exploits the temporal profile of the field to generate phase-controllable transport. Calculations in a trans- polyacetylene oligomer coupled to metallic leads indicate that the mechanism is highly efficient and robust to ultrafast electronic dephasing processes induced by vibronic couplings.