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arXiv 0709.0771cond-mat.mes-hallcond-mat.other
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强整形脉冲激励下分子隧道结中的光感应电流理论

Theory of light-induced current in molecular-tunneling junctions excited with intense shaped pulses

B. D. Fainberg, M. Jouravlev, A. Nitzan

摘要:

本文描述了分子隧道结中强光脉冲引起的光感生感应电流理论。我们考虑一个分子桥表示其最高占用和最低未占用的水平,HOMO和LUMO,分别。我们考虑到两种类型的分子和金属引线之间的耦合:电子转移,产生净电流的偏置结和能量转移之间的分子和电子空穴激发的引线。使用马尔可夫近似,我们推导出一个封闭的系统的方程的期望值的相关变量:人口和分子极化是二元的,和激子人口是四元的湮灭和创建运营商的电子在分子状态。我们提出了一种利用啁啾脉冲增强无偏结中电荷转移的光学控制方法,其中桥接分子的特征在于强电荷转移跃迁。所得到的动力学方程的近似解析解支持的完整的数值解。当不存在分子与电子-空穴激发之间的能量转移时,线性啁啾脉冲诱导电荷转移的光学控制问题可以归结为朗道-齐纳跃迁的衰减问题。当啁啾相对于电子转移速率快时,朗道理论得到恢复。提出的控制机制是潜在的有用的开发新的光电单电子器件的光学门控基于分子纳米结。

英文摘要:

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.

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