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These experiments investigate the competition between C–C and C–Br bond fission in bromoacetone excited in the 1[n(O),π*(C=O)] absorption, elucidating the role of molecular conformation in influencing the probability of adiabatically traversing the conical intersection along the C–C fission reaction coordinate. In the first part of the paper, measurement of the photofragment velocity and angular distributions with a crossed laser‐molecular beam time‐of‐flight technique identifies the primary photofragmentation channels at 308 nm. The time‐of‐flight spectra evidence two dissociation channels, C–Br fission and fission of one of the two C–C bonds, BrH2C–COCH3. The distribution of relative kinetic energies imparted to the C–Br fission and C–C fission fragments show dissociation is not occurring via internal conversion to the ground electronic state and allow us to identify these channels in the closely related systems of bromoacetyl‐ and bromopropionyl chloride.In the second part of the work we focus on the m...

the journal of chemical physics

Competing C–Br and C–C bond fission following 1[<i>n</i>(O),π*(C=O)] excitation in bromoacetone: Conformation dependence of nonadiabaticity at a conical intersection

Competing C–Br and C–C bond fission following 1[n(O),π*(C=O)] excitation in bromoacetone: Conformation dependence of nonadiabaticity at a conical intersection