Full characterization and optimization of a femtosecond ultraviolet laser source for time and angle-resolved photoemission on solid surfaces

A novel experimental apparatus for time and angle-resolved photoemission on solid surfaces is presented. A 6.28 eV laser source operating at 250 kHz repetition rate is obtained by frequency mixing in nonlinear beta barium borate crystals. This UV light source has a high photon flux of 10(13) photons/s with relatively low number of photons/pulse so that Fermi surface mapping over a wide region of the Brillouin zone is possible while mitigating space charge effects. The UV source has been fully characterized spatially, spectrally, and temporally. Its potential for time and angle-resolved photoemission is demonstrated through Fermi surface mapping and photoexcited electron dynamics in Bismuth. True femtosecond time resolution <65 fs is obtained while the energy resolution of 70 meV appears to be mainly limited by the laser bandwidth.