Frequency Combs for Spectroscopy in the Vacuum Ultraviolet

Abstract

This dissertation explores frequency comb spectroscopy and, in particular, its extension to the vacuum-ultraviolet (VUV) and extreme-ultraviolet (XUV) wavelength regimes through a technique called intracavity high harmonic generation (IHHG). By combining the techniques of passive pulse amplification in an enhancement cavity with high harmonic generation, IHHG enables the direct conversion of near-infrared radiation to the VUV/XUV while still maintaining the underlying comb structure .As part of this work, a series of numerical simulations was performed to investigate the plasma that is formed in the IHHG process and its implications for the resulting VUV comb. It was demonstrated that a fundamental limitation to the performance of IHHG experiments is due to the single-pass ionization phase shift acquired by the pulse circulating in the enhancement cavity. Furthermore, we showed that a static background plasma accumulates between pulses and complicates cavity stabilization. Insights gained from the simulations led to the development of a novel pump-probe technique using the enhancement cavity that allowed a direct measurement of the intracavity plasma and its decay dynamics in real-time. Because the plasma lifetime plays such a crucial role in the operation of these cavities, it was important to have a method to test ways of reducing it. To build on our initial IHHG results showing record-level powers in the XUV, we implemented a fully phase-coherent dual comb spectrometer consisting of two identical IHHG systems operating in parallel. The system is designed for precision spectroscopy in the VUV and is based on a pair of homemade ytterbium fiber lasers that use a parabolic amplification scheme to achieve 80 fs pulses after amplification to 50 W of average power. Initial dual comb data showing system performance at the fundamental frequency and third harmonic are presented.