UV-Driven Harmonic Generation for Time-Resolved Photoelectron Spectroscopy of Polyatomic Molecules

A single-order harmonic pulse in the vacuum-ultraviolet (VUV) is highly desirable for time-resolved photoelectron spectroscopy (TRPES) of polyatomic molecules. A high-power 9th harmonic of a Ti:sapphire laser (hv = 14 eV) is obtained using a UV driving laser at 270 nm (the 3rd harmonic). We describe our recent efforts to develop VUV TRPES combined with UV-driven harmonic generation, and present a few representative results from our recent TRPES studies