New Laser Techniques for Time-Resolved Spectroscopy

A novel spectroscopic tool is presented for measuring the incoherent resonance decay (IRD) of selectively (6 MHz) prepared electronic states. The method utilizes electro-optic switching of a single laser mode that is on or off resonance with respect to the homogeneous molecular packets in the excited ensemble. The technique is applied to a variety of systems: gases at low and high pressures, molecular beams, and solids at low temperatures. The coherent transient of solids observed in the forward direction of the laser gives the phase memory (optical T2 processes) while the IRD measures directly the radiative and radiationless decay (optical T 1 processes), and the optical transition moment between the ground state and the prepared electronic state. The theory of coherent and incoherent states is also given, and related to the different aspects of time-resolved spectroscopy of molecular beams and solids.