| This work involves a series of experiments using the coherent properties of ultrafast lasers. First, vibrational and rotational spectroscopy of the N2O4 molecule is examined. The non-resonant four wave mixing rotational coherence spectroscopy method, both homodyne and heterodyne detected, is used to investigate both short time ground state vibrational dynamics and long time scale rotational dynamics. Accurate rotational constants, vibrational frequencies and anharmonicities are measured for the N2O 4 molecule.; Rotational coherence spectroscopy is also used to investigate the effect of high intensity laser pulses on sample molecules. Both alignment and deformation are observed, in fields from 1010 W/cm2 to 10 13 W/cm2. These effects are verified by time of flight mass spectrometry. Resonant four wave mixing spectroscopy is used to measure the decoherence cross sections for the coherence between the X(1Sigma g+) and B(3pi0u+) states of I2 in a series of buffer gas molecules. Lennard-Jones parameters are extracted for He, Ar, C3H8, N2, and O2. Finally, Multiphoton intrapulse interference is examined in an effort to simplify the search space typically investigated by pulse shapers. The concept of Binary Phase Shaping for two photon excitation is investigated as a coherent control method. |
