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Phys. Rev. Lett. 99, 126802 (2007) [4 pages]

Robust Ultrafast Currents in Molecular Wires through Stark Shifts

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Ignacio Franco1, Moshe Shapiro2, and Paul Brumer1
1Chemical Physics Theory Group, Department of Chemistry, and Center for Quantum Information and Quantum Control, University of Toronto, Toronto, Ontario, Canada
2Chemical Physics Department, The Weizmann Institute, Rehovot, Israel, and Departments of Chemistry and Physics, The University of British Columbia, Vancouver, British Columbia, Canada

Received 4 June 2007; published 17 September 2007

A novel way to induce ultrafast currents in molecular wires using two incident laser frequencies, ω and 2ω, 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.

© 2007 The American Physical Society

URL:
http://link.aps.org/doi/10.1103/PhysRevLett.99.126802
DOI:
10.1103/PhysRevLett.99.126802
PACS:
85.65.+h, 72.10.Di, 73.63.−b, 78.20.Jq