Spectroscopic studies in the picosecond domain with synchronously mode-locked dye lasers

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Abstract
Synchronous mode locking of two dye lasers was employed to obtain pairs of independently tunable picosecond pulses that were precisely synchronized in time. Overlapped pulses in strontium vapor were used to generate tunable picosecond pulses in the vacuum uv. The tunability was employed to study resonant enhancement of a four‐wave parametric process by the 4d6p autoionizing resonance. Mutually separated pulses were employed to measure the build‐up and decay of coherence for a two‐quantum excited state. The decay was found to be faster than theoretical predictions that assume only velocity dephasing.