The possibility that chemical reactions may be controlled by tailored femtosecond laser pulses has inspired recent studies that take advantage of their short pulse duration, comparable to intramolecular dynamics, and high peak intensity to fragment and ionize molecules. Among them are dreams, breakthroughs and disappointments. In this dissertation, the results from a comprehensive study are presented for isolated molecules interact with shaped near-IR laser pulses with peak intensities ranging from 1013 to 1016 W/cm2. Important lessons were learned for laser control chemistry under such conditions from exhaustive evaluation of hundreds of thousands of experiments from 16 compounds. Its potential applications in analytical chemistry are also discussed. Results studying the dynamics occurring soon after isolated molecules interact with an intense non-resonant laser field are also presented in this dissertation. This study reveals dynamics that take place over a range that extends through four orders of magnitude in time, which provide information about how molecules interact with intense laser fields and how pulse shaping influences the yield of different fragment ions.
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