External field control of charge transmission through single molecules: Switching effects and transient currents

摘要

Net electron transfer through a single molecule attached to nano electrodes can undergo a pronounced change by resonant optical excitation. Caused by the population of excited electronic states of the molecule new transmission channels are opened which alter the current–voltage characteristics of the junction. This recent suggestion is further investigated here by studying the transient behavior of the current if the external laser pulse excitation is switched-on and -off within a certain time-interval. The computations concentrate on the case of weak and intermediate molecule–lead coupling. They are carried out in using rate equations which govern the populations of the different electron-vibrational states of the molecule being in its neutral or charged state. The interrelation of the switching-time and the time of charging and discharge of the molecule as well as of the time of vibrational relaxation is demonstrated by working in a switching-time range of some hundreds fs up to about 50 ps.