Laser-induced currents along molecular wire junctions

Details Laser-induced currents along molecular wire junctions Laser-induced currents along molecular wire junctions

2008-05-20

arxiv.org/abs/0805.3187v1

Physics

Quantum Physics

14 pages, 10 figures. Accepted in J. Chem. Phys

Scientific paper

10.1063/1.2940796

The treatment of the previous paper is extended to molecular wires. Specifically, the effect of electron-vibrational interactions on the electronic transport induced by femtosecond $\omega+2\omega$ laser fields along unbiased molecular nanojunctions is investigated. For this, the photoinduced vibronic dynamics of trans-polyacetylene oligomers coupled to macroscopic metallic leads is followed in a mean-field mixed quantum-classical approximation. A reduced description of the dynamics is obtained by introducing projective lead-molecule couplings and deriving an effective Schr\"odinger equation satisfied by the orbitals in the molecular region. Two possible rectification mechanisms are identified and investigated. The first one relies on near-resonance photon-absorption and is shown to be fragile to the ultrafast electronic decoherence processes introduced by the wire's vibrations. The second one employs the dynamic Stark effect and is demonstrated to be highly efficient and robust to electron-vibrational interactions.

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