| The work presented in this dissertation describes the use of shaped femtosecond laser pulses to control the outcome of nonlinear optical process and thus to achieve the selectivity for multiphoton molecular transitions. This research could lead to applications in various fields including nonlinear optical spectroscopy, chemical identification, biological imaging, communications, photodynamic therapy, etc.;In order to realize accurate pulse shaping of the femtosecond laser pulses, it is essential to measure and correct the spectral phase distortion of such pulses. A method called multiphoton intrapulse interference phase scan is used to do so throughout this dissertation. This method is highly accurate and reproducible, and has been proved in this work to be compatible with any femtosecond pulses regardless of bandwidth, intensity and repetition rate of the laser. The phase control of several quasi-octave laser sources is demonstrated in this dissertation, with the generation of 4.3 fs and 5.9 fs pulses that reach the theoretically predicted transform-limited pulse duration.;The excellent phase control achieved also guarantees the reproducibility for selective multiphoton excitations by accurate phase and/or amplitude shaping. Selective two-photon excitation, stimulated Raman scattering and coherent anti-Stokes Raman scattering with a single broadband laser source are demonstrated in this dissertation. Pulse shaping is used to achieve a fast and robust approach to measure the two-photon excitation spectrum from fluorescent molecules, which provide important information for two-photon biological imaging. The selective excitation concept is also applied in the field of remote chemical identification. Detection of characteristic Raman lines for several chemicals using a single beam coherent anti-Stokes Raman scattering spectroscopy from a 12 meter standoff distance is shown, providing a promising approach to standoff detection of chemicals, hazardous contaminations, and explosives. |
