Advancements in laser technology over the last decades have allowed compression of laser light pulses to few-femtosecond durations. To obtain even shorter pulses, a new mechanism was required. The discovery of high-order harmonic generation, a non-perturbative nonlinear optical process, allowed the conversion of ultrafast laser pulses into a coherent extreme ultraviolet light (XUV) source of attosecond pulses. The attosecond XUV light source, which corresponds to the natural time and energy scales of electron motion in matter, has provided a tool to capture the fastest dynamics in atoms, molecules, and solids and opened the field of attosecond science. However, the generation of isolated attosecond pulses has traditionally required state-of-the-art, few-cycle Ti:Sapphire laser systems and advanced facilities, which limit its applications in other science fields. Recently, ytterbium-doped solid state and fiber lasers have become attractive tools for ultrafast science and industrial applications, due largely to their prospects for scaling to high peak- and average power and their turn-key operation. However, applying these sources as driving lasers for attosecond pulse generation is challenging due to their long pulse durations. In this dissertation, I discuss progress towards attosecond time-resolved experiments using a turn-key Yb:KGW laser amplifier. First, we overcome the unfavorable long laser pulse duration by generating broadband, coherent supercontinuum spectra via nonlinear propagation in a molecular gas-filled hollow-core fiber. The pulses are compressed to sub-two-cycle durations using a two-channel field synthesizer, and methods to mitigate thermal effects at high average powers are explored. The laser pulses are characterized using a new single-shot waveform measurement technique based on multiphoton excitation in a solid medium, and we demonstrate its applicability to studies of attosecond field reshaping during nonlinear propagation. Finally, a source of isolated iv attosecond pulses based on a two-stage hollow-core fiber compressor with carrier-envelope phase stabilization and temporal gating is proposed.

Complex optical pulse shapes are typically generated from ultrashort laser pulses by manipulating the optical spectrum of the input pulses. This generates complex but periodic time-domain waveforms. Optical Arbitrary Waveform Generation (OAWG) builds on the techniques of ultrashort pulse-shaping, with the goal of making non-periodic, truly arbitrary optical waveforms. Some applications of OAWG are coherently controlling chemical reactions on a femtosecond time scale, improving the performance of LADAR systems, high-capacity optical telecommunications and ultra wideband signals processing. In this work, an array of Vertical Cavity Surface Emitting Lasers (VCSELs) are used as modulators, by injection-locking each VCSEL to an individual combline from an optical frequency comb source. Injection-locking ensures that the VCSELs' emission is phase coherent with the input combline, and modulating its current modulates mainly the output optical phase. The multi-GHz modulation bandwidth of VCSELs updates the output optical pulse shape on a pulse-to-pulse time scale, which is an important step towards true OAWG. In comparison, it is about a million times faster than the liquid-crystal modulator arrays typically used for pulse shaping! Novel components and subsystems of Optical Arbitrary Waveform Generation (OAWG) are developed and demonstrated in this work. They include: 1. Modulators An array of VCSELs is packaged and characterized for use as a modulator for rapid?update pulse?shaping at GHz rates. The amplitude and phase modulation characteristics of an injection-locked VCSEL are simultaneously measured at GHz modulation rates. 2. Optical Frequency Comb Sources An actively mode-locked semiconductor laser was assembled, with a 12.5 GHz repetition rate, ~ 200 individually resolvable comblines directly out of the laser, and high frequency stability. In addition, optical frequency comb sources are generated by modulation of a single frequency laser. 3. High-resolution optical spectral demultiplexers The demultiplexers are implemented using bulk optics, and are used to spatially resolve individual optical comblines onto the modulator array. 4. Optical waveform measurement techniques Several techniques are used to measure generated waveforms, especially for spectral phase measurements, including multi-heterodyne phase retrieval. In addition, an architecture for discriminating between ultrashort encoded optical pulses with record high sensitivity is demonstrated.