Ultrafast extreme ultraviolet photoemission without space charge

TL;DR

This paper demonstrates space-charge-free ultrafast XUV photoemission with high photon flux and tunability, enabling new time-resolved experiments without spectral distortions.

Contribution

The authors develop a tunable, high-repetition-rate XUV source that achieves high photon flux without space charge effects, expanding capabilities for ultrafast photoemission studies.

Findings

Achieved up to 5 nA average sample current without space charge distortions.

Delivered over 10^11 photons/sec in isolated harmonics from 18 to 37 eV.

Observed laser-assisted photoelectric effect with very low sideband amplitudes.

Abstract

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 $58 \times 100 \; \mu$m$^2$. 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 the laser-assisted photoelectric effect with sideband amplitudes as low as $6 \times 10^{-4}$, enabling time-resolved XUV photoemission experiments in a qualitatively new regime.