Date of Award
Doctor of Philosophy (PhD)
Margaret M. Murnane
Henry C. Kapteyn
High harmonic generation (HHG) is an extreme nonlinear optical process. When implemented in a phase-matched geometry, HHG coherent upconverts femtosecond laser light into coherent “X-ray laser” beams, while retaining excellent spatial and temporal coherence, as well as the polarization state of the driving laser. HHG has a tabletop footprint, with femtosecond to attosecond time resolution, combined with nanometer spatial resolution. As a consequence of these unique capabilities, HHG is now being widely adopted for use in molecular spectroscopy and imaging, materials science, as well as nanoimaging in general. In the first half of this thesis, I demonstrate high flux linearly polarized soft X-ray HHG, driven by a single-stage 10-mJ Ti:sapphire regenerative amplifier at a repetition rate of 1 kHz. I first down-converted the laser to 1.3 μm using an optical parametric amplifier, before up-converting it into the soft X-ray region using HHG in a high-pressure, phase-matched, hollow waveguide geometry. The resulting optimally phase-matched broadband spectrum extends to 200 eV, with a soft X-ray photon flux of > 106 photons/pulse/1% bandwidth at 1 kHz, corresponding to > 109 photons/s/1% bandwidth, or approximately a three orders-of-magnitude increase compared with past work. Using this broad bandwidth X-ray source, I demonstrated X-ray absorption spectroscopy of multiple elements and transitions in molecules in a single spectrum, with a spectral resolution of 0.25 eV, and with the ability to resolve the near edge fine structure.
In the second half of this thesis, I discuss how to generate the first bright circularly polarized (CP) soft X-ray HHG and also use them to implement the first tabletop X-ray magnetic circular dichroism (XMCD) measurements. Using counter-rotating CP lasers at 1.3 μm and 0.79 μm, I generated CPHHG with photon energies exceeding 160 eV. The harmonic spectra emerge as a sequence of closely spaced pairs of left and right CP peaks, with energies determined by conservation of energy and spin angular momentum. I explain the single-atom and macroscopic physics by identifying the dominant electron quantum trajectories and optimal phase matching conditions. The first advanced propagation simulations for CPHHG reveal the influence of the finite phase matching temporal window on the spectrum, as well as the unique polarization-shaped attosecond pulse train. The first tabletop XMCD measurements at the N4,5 absorption edges of Gd using this light source validate the high degree of circularity, brightness, and stability of this light source. These results demonstrate the feasibility of manipulating the polarization, spectrum and temporal shape of soft X-ray HHG by manipulating the driving laser waveform.
Finally, I present the first bright phase-matched CPHHG driven by lasers at wavelengths of 2 μm and 0.79 μm, which extends CPHHG to a broader wavelength combination and confirms the universal nature of this generation scheme. By analyzing the helicity dependent intensity asymmetry of CPHHG generated using different wavelengths and different gas targets, I show that the helicity dependent intensity asymmetry was mostly caused by the helicity dependent single-atom physics, which exhibits different behaviors for different gas targets. Moreover, the asymmetry can reverse and very interestingly, CPHHG from Ar exhibits a single helicity in the high-photon-energy region of the spectrum, which provide a convenient way to generate CPHHG with a single helicity and CP attosecond pulse trains. Finally, simple simulations and cutoff analysis of CPHHG provide guidance for generating CPHHG at higher photon energies.
Fan, Tingting, "Bright Linearly and Circularly Polarized Extreme Ultraviolet and Soft X-Ray High Harmonics for Absorption Spectroscopy" (2017). Physics Graduate Theses & Dissertations. 266.