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High-flux ultrafast extreme-ultraviolet photoemission spectroscopy at 18.4 MHz pulse repetition rate

: Saule, T.; Heinrich, S.; Schötz, J.; Lilienfein, N.; Högner, M.; Vries, O. de; Plötner, M.; Weitenberg, J.; Esser, D.; Schulte, J.; Russbueldt, P.; Limpert, J.; Kling, M.F.; Kleineberg, U.; Pupeza, T.

Volltext ()

Nature Communications 10 (2019), Art. 458, 10 S.
ISSN: 2041-1723
Zeitschriftenaufsatz, Elektronische Publikation
Fraunhofer ILT ()
Fraunhofer IOF ()

Laser-dressed photoelectron spectroscopy, employing extreme-ultraviolet attosecond pulses obtained by femtosecond-laser-driven high-order harmonic generation, grants access to atomic-scale electron dynamics. Limited by space charge effects determining the admissible number of photoelectrons ejected during each laser pulse, multidimensional (i.e. spatially or angle-resolved) attosecond photoelectron spectroscopy of solids and nanostructures requires high-photon-energy, broadband high harmonic sources operating at high repetition rates. Here, we present a high-conversion-efficiency, 18.4-MHz-repetition-rate cavity-enhanced high harmonic source emitting 5 × 105 photons per pulse in the 25-to-60-eV range, releasing 1 × 1010 photoelectrons per second from a 10-µm-diameter spot on tungsten, at space charge distortions of only a few tens of meV. Broadband, time-of-flight photoelectron detection with nearly 100% temporal duty cycle evidences a count rate improvement between two and three orders of magnitude over state-of-the-art attosecond photoelectron spectroscopy experiments under identical space charge conditions. The measurement time reduction and the photon energy scalability render this technology viable for next-generation, high-repetition-rate, multidimensional attosecond metrology.