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.
As conventional electronics approaches its ultimate limits, novel concepts of fast quantum control have been sought after. Lightwave electronics – the foundation of attosecond science – has opened a new arena by utilizing the oscillating carrier wave of intense light pulses to control electrons faster than a cycle of light. We employ atomically strong terahertz electromagnetic pulses to accelerate electrons through the entire Brillouin zone of solids, drive quasiparticle collisions, and generate high-harmonic radiation as well as high-order sidebands. The unique band structures of topological insulators allow for all-ballistic and quasi-relativistic acceleration of Dirac quasiparticles over distances as large as 0.5 μm. In monolayers of transition metal dichalcogenides, we switch the electrons’ valley pseudospin, opening the door to subcycle valleytronics. Finally, we show that lightwave electronics can be combined with ultimate atomic spatial resolution in state-selective ultrafast scanning tunneling microscopy.
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