Using a single-molecule switch, we study atom-scale light-matter interaction. First, we utilize atomically confined terahertz transients to measure and control molecular motion in real space. Based on atomically precise lightwave-driven scanning tunneling microscopy (STM), we unravel how light pulses can act as sub-picosecond atomic forces on key atoms of a molecular switch to coherently steer structural dynamics. This allows us to control a frustrated structural rotation that modulates the molecule’s switching probability. Second, we investigate near-field waveforms on extremely sub-wavelength volumes. As atomic light-matter interaction crucially depends on both the temporal evolution and the absolute strength of local fields, a parameter-free method to directly measure and calibrate atom-scale waveforms has been highly desirable. Calibrating the electric near field with a single-molecule switch, we quantitatively measure the temporal shape and amplitude of atomically confined light-field transients inside the tunneling gap of the scanning tunneling microscope.
|