Onset of decoherence: six-wave mixing measurements of vibrational decoherence on the excited electronic state of I2 in solid argon.

摘要: Pump-probe, four-wave, and six-wave mixing measurements of I2 isolated in solid argon are used to provide a clear experimental measure for the onset vibrational quantum decoherence on excited electronic state. The electronically resonant, bypass rapid dephasing, cross-correlation between two packets launched B-state. coherence survives one period motion, 400 fs, during which approximately 2000 cm(-1) energy is transferred lattice. occurs second cycle while classically coherent motion measured via pump-probe spectroscopy using same resonances continues 15 periods. This contrasted with dephasing ground surface, lasts 10(2) periods, as through time-resolved anti-Stokes Raman scattering. observables discussed time-circuit diagrams, mechanistic description derived semiclassical analysis simulations that reproduce experiments.