Investigation of vibrating-hydrogen based ultrashort molecular phase modulator

This thesis investigates the coherent phase modulation of ultrashort pulses using vibrating hydrogen as a molecular medium. Self-phase modulation in a gas-filled hollow core capillary allows the generation of highpower few-cycle pulses in the NIR. Such pulses can be used to drive high harmonic generation (HHG) to deliver attosecond duration pulses in the extreme ultraviolet and soft X-ray spectral region. While reaching unrivalled pulse durations (down to 67 as), these sources have characteristically low efficiencies. The pump-probe spectroscopy community would greatly benefit from brighter short wavelength sources with sub-5 fs duration. In this work I apply Amplified RamaN Impulsive Excitation for Molecular Phase Modulation (ARNIEMPM), a multiple pulse scheme, to coherently prepare vibrating hydrogen molecules and exploit them for the phase modulation of ultrashort pulses. The preparation of the molecular motion is performed via impulsive stimulated Raman scattering and transient stimulated Raman scattering. The generated in-phase motion of molecules creates an oscillating optical polarizability in the medium which can be exploited by a probe pulse propagating through it, acting as a 125THz frequency phase modulator, the fastest among molecular media. This technique has the potential to provide bright, isolated subfemtosecond duration ultra-violet (UV) pulses via spectral broadening of broadband pulses. I experimentally investigate the preparation of the molecular motion against multiple experimental parameters. I then demonstrate the molecular phase modulation of ultrashort broadband probes in the near-infrared (NIR) and UV via a degenerate interferometric scheme. I used a waveguide to increase the interaction length of the process and reduce the energy requirements for the medium preparation. This allowed the use of a single laser system to generate all the required pulses, which are largely diverse in terms of wavelength, duration and power. Additionally, I present a novel technique named Attosecond Resolved Interferometric Electric-field Sampling (ARIES), which is capable of directly measuring the waveform of arbitrary pulses with attosecond resolution. This technique is based on high-harmonic generation (HHG) acting as a temporal gate for an applied secondary field, and tracking its electric field amplitude as a shift in the HHG cut-off frequency. I present experimental demonstration of a pulse waveform measurement by accurately retrieving a know inserted variation in dispersion and carrier-envelope-phase. A theoretical calculation of the technique applicability over a wide spectral range is also presented.