Tuning time and energy resolution in time-resolved photoemission spectroscopy with nonlinear crystals

Abstract

Time-and angle-resolved photoemission spectroscopy is a powerful probe of electronic band structures out of equilibrium. Tuning time and energy resolution to suit a particular scientific question has become an increasingly important experimental consideration. Many instruments use cascaded frequency doubling in nonlinear crystals to generate the required ultraviolet probe pulses. We demonstrate how calculations clarify the relationship between laser bandwidth and nonlinear crystal thickness contributing to experimental resolutions and place intrinsic limits on the achievable time-bandwidth product. Experimentally, we tune time and energy resolution by varying the thickness of nonlinear β-BaB2O4 crystals for frequency up-conversion, providing for a flexible experiment design. We achieve time resolutions of 58 to 103 fs and corresponding energy resolutions of 55 to 27 meV.