Tracking Electron Dynamics of Single Molecules in Scanning Tunneling Microscopy Junctions with Laser Pulses.

On the basis of real-time simulations, we devise a method to extend the capability of scanning tunneling microscopy (STM) to track the electronic dynamics of molecules on a material's surface with the ultrafast temporal resolution of laser pulses. The intrinsic mechanism of visualization of electronic dynamics by measuring tunneling charge is attributed to the interference between the electronic oscillations stimulated by pump and probe pulses. The charge-transfer rate from molecule to the surrounding environment can be estimated with the decay time of electronic dynamics, which can also be detected by measuring the tunneling charge across the STM junction. Moreover, it is found that the tunneling charge can be varied precisely by changing the carrier-envelope phase (CEP) of the pulses, and this phase-dependence of tunnelling diminishes as the duration of incident laser pulses increases. The proposed scheme provides an alternative means for visualization of electron dynamics of single molecules by measuring tunnelling charges.