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 $\omega$ vs. $2\omega$ 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 $\omega +2\omega$ 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 fs 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.

14 pages, 13 figs. Accepted in J. Chem. Phys

References in corpus (4)

• Vibrational effects in laser driven molecular wires
• Rectification of laser-induced electronic transport through molecules
• Robust ultrafast currents in molecular wires through Stark shifts
• Minimum requirements for laser-induced symmetry breaking in quantum and classical mechanics

Cited by in corpus (5)

• Computational Methodologies and Physical Insights into Electronic Energy Transfer in Photosynthetic Light-Harvesting Complexes
• Incoherent Excitation of Thermally Equilibrated Open Quantum Systems
• Laser-induced currents along molecular wire junctions
• Long-lived oscillatory incoherent electron dynamics in molecules: trans-polyacetylene oligomers
• Quantifying fermionic decoherence in many-body systems