Nonlinear optics in non-equilibrium microplasmas

This dissertation details the nature of subnanosecond laser-induced microplasma dynamics, particularly concerning the evolution of the electron temperature and concentration. Central to this development is the advent of a femtosecond four-wave mixing (FWM) spectroscopic method. FWM (in the form of coherent anti-Stokes Raman scattering (CARS)) measurements are performed on the fundamental oxygen vibrational transition. An analytical expression is provided that accounts for the resonant and nonresonant contributions to the CARS signal generated from the interaction of broadband pump and Stokes pulses. The inherent phase mismatch is also accounted for, resulting in quantitative agreement between experiment and theory. FWM is then used to measure the early-time electron dynamics in the noble gas series from He to Xe following irradiation by an intense (1014 Wcm-2) nonresonant 80 fs laser pulse. An electron impact ionization cooling model is presented to determine the evolution of electron kinetic energies following ionization. Kinetic energies are predicted to evolve from > 20 eV to < 1 eV in the first 1.5 ns. The initial degree of ionization is determined experimentally via measurement of the Bremsstrahlung background emission, and modeled with a modified ADK theory based on tunnel ionization. Combined, these two descriptions account for the evolution of both the electron temperature and concentration and provide quantitative agreement with the FWM measurements. The model is further tested with measurements of the gas pressure and pump laser intensity on the electron dynamics. The FWM experiments are concluded with a qualitative discussion of dissociative recombination dynamics occurring in molecular microplasmas. The microplasma environment is used as a source for the generation of two-level systems in the excited state manifold of atomic oxygen and argon. These two-level systems are coupled using moderately intense ∼1 ps near-infrared (and near-resonant) pulses, resulting in Rabi sidebands with unprecedentedly large shifts in excess of 90 meV. A time-dependent generalized Rabi-cycling model is developed to account for the time-dependence of the laser electric field and subsequently the Rabi frequency. The Rabi radiation is determined to be coherent and tunable (up to 200 meV), providing a new method for ultrashort pulse generation. The dependence of the spectral positions of the Rabi sidebands on laser intensity affords the opportunity to simultaneously determine the ratios of transition dipole moments for the states accessed