The technique of infrared multiphoton ionization was used to obtain state specific internal conversion rates in CrO2Cl2. Using tunable 10 ps dye laser pulses, different vibrational states in theB1manifold were excited and the energy relaxation was monitored by an IR ps laser pulse. The relaxation can be characterized by a fast component, which is due to internal conversion to the1A1state, and a slow component, which is due to cooling of the vibrationally hot1A1ground state. The nonradiative energy transfer rate changes by almost three orders of magnitude for an excess vibrational energy change of merely 550 cmminus;1. The possibility of state specific pumping of1A1is also pointed out.
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