title: Femtosecond dynamics and laser control of charge transport in trans-polyacetylene.
abstract: The induction of dc electronic transport in rigid and flexible trans-polyacetylene oligomers according to the omega versus 2omega coherent control scenario is investigated using a quantum-classical mean field approximation. The approach involves running a large ensemble of mixed quantum-classical trajectories under the influence of omega+2omega laser fields and choosing the initial conditions by sampling the ground-state Wigner distribution function for the nuclei. The vibronic couplings are shown to change the mean single-particle spectrum, introduce ultrafast decoherence, and enhance intramolecular vibrational and electronic relaxation. Nevertheless, even in the presence of significant couplings, limited coherent control of the electronic dynamics is still viable, the most promising route involving the use of femtosecond pulses with a duration that is comparable to the electronic dephasing time. The simulations offer a realistic description of the behavior of a simple coherent control scenario in a complex system and provide a detailed account of the femtosecond photoinduced vibronic dynamics of a conjugated polymer.
authors.affiliation: Chemical Physics Theory Group, Department of Chemistry and Center for Quantum Information and Quantum Control, University of Toronto, Toronto, Ontario M5S 3H6, Canada.
authors.forename: Ignacio
authors.initials: I
authors.lastname: Franco
authors.forename: Moshe
authors.initials: M
authors.lastname: Shapiro
authors.forename: Paul
authors.initials: P
authors.lastname: Brumer
mesh_terms: D004583:Electrons; D007834:Lasers; D008956:Models, Chemical; D009038:Motion; D010777:Photochemistry; D053279:Polyynes / Q000737:chemistry*; D013995:Time; D014732:Vibration
chemical_list: D053279:Polyynes