The first vibronically resolved measurement of correlated-product-state distributions in ultraviolet photodissociation: Ketene at 308 nm

A new method is demonstrated which allows derivation of elements of the correlated-product-state distribution matrix in photodissociation. The method relies on quantum-state-specific, time-of-flight measurements, which were successfully carried out on CO produced in ketene photolysis at 308 nm. Such time-of-flight data exhibits well-defined peaks dictated by the CH2 internal state distribution occurring in coincidence with the chosen CO quantum state. For two rovibrational states of CO, peaks corresponding to the 1A1(0,0,0), 1A1(0,1,0), and 3B1 vibronic states of the CH2 fragment were clearly resolved.