Physics – Condensed Matter – Mesoscale and Nanoscale Physics
Scientific paper
2007-09-06
Phys. Rev. B 76, 245329 (2007)
Physics
Condensed Matter
Mesoscale and Nanoscale Physics
14 pages, 7 figures; submitted to PRB
Scientific paper
10.1103/PhysRevB.76.245329
A theory for light-induced current by strong optical pulses in molecular-tunneling junctions is described. We consider a molecular bridge represented by its highest occupied and lowest unoccupied levels, HOMO and LUMO, respectively. We take into account two types of couplings between the molecule and the metal leads: electron transfer that gives rise to net current in the biased junction and energy transfer between the molecule and electron-hole excitations in the leads. Using a Markovian approximation, we derive a closed system of equations for the expectation values of the relevant variables: populations and molecular polarization that are binary, and exciton populations that are tetradic in the annihilation and creation operators for electrons in the molecular states. We have proposed an optical control method using chirped pulses for enhancing charge transfer in unbiased junctions where the bridging molecule is characterized by a strong charge-transfer transition. An approximate analytical solution of the resulting dynamical equation is supported by a full numerical solution. When energy transfer between the molecule and electron-hole excitations in the leads is absent, the optical control problem for inducing charge transfer with linearly chirped pulse can be reduced to the Landau-Zener transition to a decaying level. When chirp is fast with respect to the rate of the electron transfer, the Landau theory is recovered. The proposed control mechanism is potentially useful for developing novel opto-electronic single-electron devices with optical gating based on molecular nanojunctions.
Fainberg Boris D.
Jouravlev Mikhail
Nitzan Abraham
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