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Image potential states are well established surface states of metallic films [1]. For a single metallic nanostructure these surface states can be localized in the near-field arising from illumination by a strong laser field. Thus single metallic nanostructures offer the unique possibility to study quantum systems with both high spatial and ultrafast temporal resolution. Here, we investigate the dynamics of Rydberg states localized to a sharp metallic nanotaper.
For this purpose we realized a laser system delivering few-cycle pulses tunable over a wide wavelength range [2]. Pulses from a regenerative titanium:sapphire amplifier generate a white light continuum, from which both a proportion in the visible and in the infrared are amplified in two non-collinear optical parametric amplification (NOPA) stages. Difference frequency generation (DFG) of both stages provides pulses in the near-infrared.
With a precisely delayed sequence of few-cycle pulses centered around 600 nm (NOPA#1 output) and 1600 nm (DFG output) we illuminate the apex of a sharply etched gold tip. Varying the delay we observe an exponential decay of photoemitted electrons with a distinctly asymmetric decay length on both sides, indicating the population of different states. Superimposed on the decay is a clearly discernible quantum beat pattern with a period of <50 fs, which arises from the motion of Rydberg photoelectrons bound within their own image potential. These results therefore constitute a step towards controlling single electron wavepackets released from a gold tip opening up fascinating perspectives for applications in ultrafast electron microscopy [3].
[1] Hofer, U. et al. Science 277, 1480 (1997)
[2] Vogelsang, J., Robin J. et al. Opt. Express 22, 25295 (2014)
[3] Petek, H. et al. ACS Nano 8, 5 (2014)
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