High repetition rate Time-Resolved VUV ARPES at 10.8 eV photon energy

TL;DR

This paper introduces a high-repetition-rate, high-resolution VUV photon source at 10.8 eV for time-resolved ARPES, enabling detailed studies of electronic dynamics in complex materials with minimal space-charge effects.

Contribution

A novel method to generate 10.8 eV photon pulses at 1-4 MHz with high energy resolution and low space-charge effects, suitable for advanced TR-ARPES experiments.

Findings

Achieved 26 meV energy resolution at 700 fs time resolution.

Demonstrated high count rates and space-charge free operation.

Successfully measured electronic band structures of WTe₂ and Bi₂Se₃.

Abstract

The quest for mapping the femtosecond dynamics of the electronic band structure of complex materials via Time- and Angle-Resolved Photoelectron Spectroscopy (TR-ARPES) over their full First Brillouin Zone is pushing the development of schemes to efficiently generate ultrashort photon pulses in the VUV-range of photon energies. At present, the critical aspect is to combine a high photon energy with high photoemission count rates and a small pulse-bandwidth, necessary to achieve high energy resolution in ARPES, while preserving a good time resolution and mitigating space-charge effects. Here we describe a novel approach to produce light pulses at 10.8 eV, combining high repetition rate operation (1-4 MHz), high energy resolution ($\sim26$ meV) and space-charge free operation, with a time-resolution of $\sim$700 fs. These results have been achieved by generating the 9th harmonic of a Yb fiber laser, through a phase-matched process of third harmonic generation in Xenon of the laser third harmonic. The full up-conversion process is driven by a seed pulse energy as low as 10 $\mu$J, hence is easily scalable to multi-MHz operation. This source opens the way to TR-ARPES experiments for the investigation of the electron dynamics over the full first Brillouin zone of most complex materials, with unprecedented energy and momentum resolutions and high count rates. The performances of our setup are tested in a number of experiments on WTe$_2$ and Bi$_2$Se$_3$, of which we measure the electronic band structure in energy, two-dimensional momentum and time.