Recent IR experiments on the time dependent vibrational and rotational response of CN-ions in crystals indicate that the vibrational dynamics of this diatomic molecule in solids leads to unexpected lasing behavior. If other diatomic defects in crystals have properties related to CN- then solid state vibrational lasers could be practical for a variety of applications in the infrared and far-infrared spectral regions. One fundamental experimental problem has been the lack of coincidences between near-IR color center laser pumps and the overtone frequencies of molecules which can be doped into crystals. The discovery by the PI that nonresonant UV laser radiation can be used to pump the vibrational manifold of CN- opens up another avenue through which the IR radiative properties of molecules in solids can be studied. The interfacing of a pulsed UV excimer laser to an ultrahigh resolution fourier-transform infrared spectrometer will provide a new efficient type of time resolved vibrational spectroscopy which can be used to explore multilevel IR energy transfer of molecules in the solid state. For the examination of complex molecules with subnsecond relaxation times the fourier- transform infrared spectrometer will be used in a different mode to time analyze the delay between picosecond pulses in the measurement of fast saturable absorption in the anharmonic vibrator.
