"This dissertation outlines the development of several methods and techniques that enable comprehensive control of laser-matter interactions and nonlinear optical processes using shaped femtosecond pulses. Manipulation of the spectral phases and amplitudes of femtosecond laser pulses provides an effective way to adjust laser parameters, both those intrinsic to pulse generation within a laser and those induced by laser-matter interactions. When coupled with a fundamental understanding of the interactions between a laser's electric field and the molecules in the propagation media, these methods make the behavior of laser pulses predictable and allow the experimental information they carry to be extracted accurately. The ultimate motivation is to enhance the accuracy and reproducibility of spectroscopic measurements and to control nonlinear processes during light-matter interaction using shaped femtosecond pulses. Ultrafast laser systems have become one of the most important scientific tools in femtochemistry, nanoscale material science, chemical detection and sensing, and many other applications where processes occur at femtosecond (fs, 10-15 of a second) timescales or when broad laser bandwidths are required. As with any measuring instrument, it is very important to know system's exact parameters in order to make meaningful, accurate and reproducible measurements. For ultrafast lasers, these parameters are the intensities of the spectral components, the spectral phase, the temporal profile, the pulse energy, and the spatial laser beam profile. Due to broadband nature of ultrafast laser sources, they are very sensitive to propagation media: gaseous, liquid or solid matter along the paths of laser pulses to the sample, including the material of the sample itself. Optical parameters describing the propagation media, such as linear and nonlinear dispersion, and birefringence, as well as physical parameters, such as temperature and pressure, all affect laser pulse parameters. In order for measurements not to be skewed, these interactions need to be taken into account and mitigated at the time of the experiment or handled later in data analysis and simulations. Experimental results are presented in four chapters. Chapter 2 describes two topics: (1) single-shot real-time monitoring and correction of spectral phase drifts, which commonly originate from temperature and pointing fluctuations inside the laser cavity when the pulses are generated; (2) an alloptical method for controlling the dispersion of femtosecond pulses using other pulses. Chapter 3 focuses on the effects of the propagation media--how intense laser pulses modify media and how, in turn, the media modifies them back--and how these effects can be counteracted. Self-action effects in fused silica are discussed, along with some interesting and unexpected results. A method is then proposed for mitigating self-action processes using binary modulation of the spectral phases of laser pulses. Chapter 4 outlines the design of two laser systems, which are specifically tailored for particular spectroscopic applications and incorporate the comprehensive pulse control described in previous chapters. Chapter 5 shows how control of spatial beam characteristics can be applied to measurements of the mechanical motion of microscale particles and how it can potentially be applied to molecular motion. It also describes an experiment on laser-induced flow in air in which attempts were made to control the macroscopic molecular rotation of gases. My research, with a pulse shaper as the enabling tool, provides important insights into ultrafast scientific studies by making femtosecond laser research more predictable, reliable and practical for measurement and control. In the long term, some of the research methods in this thesis may help the transition of femtosecond lasers from the laboratory environment into clinics, factories, airports, and other everyday settings."--Pages ii-iii.
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