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

• Published in: Nature communications 2019-01, Vol.10 (1), p.458-10, Article 458
• Main Authors: Saule, T., Heinrich, S., Schötz, J., Lilienfein, N., Högner, M., deVries, O., Plötner, M., Weitenberg, J., Esser, D., Schulte, J., Russbueldt, P., Limpert, J., Kling, M. F., Kleineberg, U., Pupeza, I.
• Format: Article
• Language: English
• Subjects: 140/146; 639/624/1020/1095; 639/766/400/3923; Attosecond pulses; Broadband; Ejection; Electrons; Femtosecond pulsed lasers; Harmonic generations; Humanities and Social Sciences; Lasers; multidisciplinary; Photoelectric emission; Photoelectron spectroscopy; Photoelectrons; Photons; Pulse repetition rate; Repetition; Science; Science (multidisciplinary); Space charge; Spectroscopy; Spectrum analysis; State of the art; Time of flight photoelectron coincidence spectroscopy; Tungsten; Ultraviolet spectroscopy
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-019-08367-y

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 × 10 5 photons per pulse in the 25-to-60-eV range, releasing 1 × 10 10 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. Space charge effects can distort the results of photoelectron spectroscopic measurements, and usually limit the allowable photon flux in an experiment. Here, the authors present an 18.4 MHz repetition rate high harmonic source in the 25–60 eV range, with a large count rate improvement over state-of-the-art attosecond setups under identical space charge conditions.