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Issue 19, 2011
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Laser pulse induced transient currents through a single molecule

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Laser pulse control of electron transfer through a single molecule attached to nano electrodes is demonstrated theoretically by concentrating on the case of weak and intermediate molecule-lead coupling. A rate equation description is used to determine the populations of the different electron-vibrational states of the molecule in its neutral or charged state. Caused by the photoinduced population of excited electronic states new transmission channels are opened which change the current through the molecular junction. The transient behavior of the current is studied if the external laser pulse excitation is switched on and off or if a pulsed excitation is applied. Pulse durations of some hundreds of fs up to 50 ps are considered. Within this computational scheme the interrelation of characteristic times of charging, discharge, vibrational relaxation, and the turn on and off of the photoexciation is demonstrated. Possible self-stabilization of an excited junction state is found. Some estimates of potential effects of plasmon excitations in the leads are also given. To have a quantity available which offers direct experimental access to the transient state of the junction the time and frequency resolved photo emission spectrum of the molecule is calculated.

Graphical abstract: Laser pulse induced transient currents through a single molecule

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Publication details

The article was received on 04 Nov 2010, accepted on 11 Apr 2011 and first published on 18 Apr 2011

Article type: Paper
DOI: 10.1039/C0CP02399J
Citation: Phys. Chem. Chem. Phys., 2011,13, 8755-8768
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    Laser pulse induced transient currents through a single molecule

    L. Wang and V. May, Phys. Chem. Chem. Phys., 2011, 13, 8755
    DOI: 10.1039/C0CP02399J

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