Ultrafast Laser-Induced Isomerization Dynamics in Acetonitrile.

Isomerization induced by laser ionization in acetonitrile (CHCN) was investigated using pump-probe spectroscopy in combination with ion-ion coincident Coulomb explosion imaging. We deduced five primary channels indicating direct C-C breakup, single and double hydrogen migration, and H and H dissociation in the acetonitrile cation. Surprisingly, the hydrogen-migration channels dominate over direct fragmentation.