Ultrafast time- and angle-resolved photoemission spectroscopy with widely tunable probe photon energy of 5.3-7.0 eV for investigating dynamics of three-dimensional materials.

Time- and angle-resolved photoemission spectroscopy (TrARPES) is a powerful technique for capturing the ultrafast dynamics of charge carriers and revealing photo-induced phase transitions in quantum materials. However, the lack of widely tunable probe photon energy, which is critical for accessing the dispersions at different out-of-plane momentum k in TrARPES measurements, has hindered the ultrafast dynamics investigation of 3D quantum materials, such as Dirac or Weyl semimetals. Here, we report the development of a TrARPES system with a highly tunable probe photon energy from 5.3 to 7.0 eV. The tunable probe photon energy is generated by the fourth harmonic generation of a tunable wavelength femtosecond laser source by combining a β-BaBO crystal and a KBeBOF crystal. A high energy resolution of 29-48 meV and time resolution of 280-320 fs are demonstrated on 3D topological materials ZrTe and SbTe. Our work opens up new opportunities for exploring ultrafast dynamics in 3D quantum materials.