The challenge is the development of predictive abilities of the extent to which the chemical reaction dynamics in one phase provides insights into the same process in the other phase. We will compare the nuclear and electronic motion occurring during the initial 200-fs photochemical dynamics in the gas and liquid phases. Using the same technique of dispersed transient absorption with 30 fs excitation UV pulses and broadband probing, we will focus on photodissociation of small polyhalogenated molecules. These molecules also exhibit competing novel types of reaction dynamics, which have importance in atmospheric and environmental chemistry, in particular, direct isomerization reactions with the formation of a product halogen-halogen bond and roaming. We will demonstrate the application of the same dispersed ultrafast transient absorption methodology to different classes of molecules in the gas phase and solution. This enables a detailed comparison of the experimental observables in the liquid and gas phases without facing the difficulties when comparing results obtained using different, phase-specific experimental methods.

The comparison of the sub-200 fs gas- and liquid-phase photochemical dynamics from dispersed continuum-probe ultrafast transient absorption experiments

ACS Fall 2021

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