Abstract
We consider the extension of ultrafast laser alignment schemes to surface-adsorbed molecules, where the laser field coerces the molecule to reorient itself relative to the surface. When probed by a scanning tunneling microscope tip, this reorientation modifies the tip-molecule distance, and thus the tunneling current, suggesting a route to an ultrafast, nanoscale current switch. In addition to exploring the controllability of adsorbed molecules by moderately intense laser fields and discussing the fundamental differences of alignment behavior between surface-adsorbed molecules and gas phase molecules, we computationally investigate the quality of orientation with respect to field intensity, field duration, and the location of the tip. Overall, the molecule moves directly to its oriented configuration, which is reasonably insensitive to the tip location. These results collectively suggest the efficacy of using laser alignment schemes to control electron transport through junctions.