The work presented in this thesis describes the operation, characterisation and optimisation of a colliding-pulse modelocked (CPM) dye laser. A method of pulse analysis has been developed which is capable of determining the shape and chirp of the output pulses to a first approximation. It involves an iterative pulse-fitting to intensity autocorrelation, interferometric autocorrelation and spectral measurements. The use of a four-prism sequence for intracavity dispersion compensation in a CPM dye laser resulted in pulse durations of 40-50fs. However, operating the laser close to the instability regime so as to obtain strong focusing in the absorber dye jet enabled pulse durations as short as 19fs to be obtained. A detailed empirical study of the dispersion- compensated laser, together with a theoretical and experimental chirp analysis, indicated the presence of strong phase shaping arising from a net positive self-phase modulation, which was attributed to the optical Kerr effect occurring in the absorber dye solvent. Various modes of operation were observed, including unidirectional lasing and a higher- order solitonlike regime. The results of pulse-fitting were found to yield strong evidence for pulse asymmetry, the pulse profiles corresponding closely to an asymmetric sech2 pulse function with a longer leading edge. A computer simulation of the CPM dye laser provided a comprehensive understanding of the underlying pulse shaping dynamics of this system, elucidating fully the experimental behaviours observed, as well as providing a clear strategy for further optimisation of the laser. In particular, optimal performance was found to depend on strong amplitude and strong phase shaping, minimal spectral filtering, the control of higher-order dispersion and the provision of extracavity dispersion compensation. An experimental study of Gires-Tournois interferometers (GTI's) for intracavity cubic phase compensation identified the key requirements for cubic phase control in the CPM dye laser, while highlighting the limitations of utilising conventional GTI structures. A subsequent theoretical analysis enabled a more suitable strategy to be devised. It involved optimising the cavity optics and using a prism system with variable prism spacing, alone or in tandem with specially tailored GTI structures. Implementation of these findings resulted in pulse durations of around 30-40fs and the elimination of pulse asymmetry, which was attributed to a residual positive cubic phase. However, the appearance of a distinctive modulation in the wings of the pulse provided strong evidence that the pulse durations from the CPM dye laser had become limited by the next higher-order dispersion term; quartic phase. To demonstrate the direct relevance of this work to the more recently developed solid- state laser systems, an alternative all-solid-state femtosecond laser has been described. Based around a Ti:sapphire gain medium, the design of this laser incorporates the essential optimising principles and techniques developed for the CPM dye laser. The proposed system utilises a low-loss, broadband semiconductor saturable absorber mirror to initiate self-modelocking and a hybrid prism-chirped-mirror scheme for broadband intracavity and extracavity quintic-phase-limited dispersion compensation. When fully optimised, it is predicted that this laser should yield pulse durations as short as 5fs.

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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.