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Laser Seminar / NCCR MUST Seminar: Ultrafast extreme ultraviolet photoemission without space charge

Date Mo, 23.07.2018 - Mo, 23.07.2018
Time 16.45
Speaker Prof. Tom Allison, Department of Chemistry, Stony Brook University, New York, USA
Location ETH Zurich, Hönggerberg Campus, HPF G6
Program Time- and Angle-resolved photoelectron spectroscopy from surfaces can be used to record the dynamics of electrons and holes in condensed matter on ultrafast time scales. However, ultrafast photoemission experiments using extreme-ultraviolet (XUV) light have previously been limited by either space-charge effects, low photon flux, or limited tuning range. In this article, we describe space-charge-free XUV photoelectron spectroscopy experiments with up to 5 nA of average sample current using a tunable cavity-enhanced high-harmonic source operating at 88 MHz repetition rate. The source delivers > 10^11 photons/s in isolated harmonics to the sample over a broad photon energy range from 18 to 37 eV with a spot size of 58 × 100 μm^2. From photoelectron spectroscopy data, we place conservative upper limits on the XUV pulse duration and photon energy bandwidth of 93 fs and 65 meV, respectively. The high photocurrent, lack of space charge distortions of the photoelectron spectra, and excellent isolation of individual harmonic orders allow us to observe laser-induced changes to the photoelectron spectrum at the 10^{-4} level in minutes of integration time, enabling time-resolved XUV photoemission experiments in a qualitatively new regime. I will discuss demonstration experiments on Au (111) and progress towards electron dynamics in molecular films.
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