Two-Color Ultrafast Photoexcited Scanning Tunneling Microscopy

We report on two-color two-photon photoexcitation of a metal surface driven by ultrafast laser pulses and detected with a scanning tunneling microscope (STM) tip as a proximate anode. Results are presented for two cases: (i) where the tip is retracted from the surface far enough to prohibit tunneling, and (ii) where the tip is within tunneling range of the surface. A delay-modulation technique is implemented to isolate the two-color photoemission from concurrent one-color two-photon photoemission and provide subpicosecond time-resolved detection. When applied with the tip in tunneling range, this approach effectively isolates the two-photon photoexcited current signal from the conventional tunneling current and enables subpicosecond time-resolved detection of the photoexcited surface electrons. The advantage of the two-color approach is highlighted by comparison with the one-color case where optical interference causes thermal modulation of the STM tip length, resulting in tunneling current modulations that are orders of magnitude larger than the current due to photoexcitation of surface electrons. By completely eliminating this interference, and thereby avoiding thermal modulation of the STM tip length, the two-color approach represents an important step toward the ultimate goal of simultaneous subnanometer and subpicosecond measurements of surface electron dynamics by ultrafast-laser-excited STM.