High Harmonic Generation Light Source with Polarization Selectivity and Sub-100-μm Beam Size for Time- and Angle-Resolved Photoemission Spectroscopy

Abstract

High-quality ultrafast light sources are critical for developing advanced time- and angle-resolved photoemission spectroscopy (TrARPES). While the application of high harmonic generation (HHG) light sources in TrARPES has increased substantially over the past decade, the optimization of the HHG probe beam size and selective control of the light polarization, which are important for TrARPES measurements, have been rarely explored. In this work, we report the implementation of high-quality HHG probe source with an optimum beam size down to 57 μm × 90 μm and selective light polarization control, together with mid-infrared (MIR) pumping source for TrARPES measurements using a 10-kHz amplifier laser. The selective polarization control of the HHG probe source allows to enhance bands with different orbital contributions or symmetries, as demonstrated by experimental data measured on a few representative transition metal dichalcogenide materials as well as topological insulator Bi 2 Se 3 . Furthermore, by combining the HHG probe source with MIR pumping at 2-μm wavelength, TrARPES on a bilayer graphene shows a time resolution of 140 fs, allowing to distinguish 2 different relaxation processes in graphene. Such high-quality HHG probe source together with the MIR pumping expands the capability of TrARPES in revealing the ultrafast dynamics and light-induced emerging phenomena in quantum materials.