Directional hydrogen migration in acetonitrile dication in asymmetric ultrashort intense laser fields

We investigate intramolecular hydrogen migration in acetonitrile dication in phase-controlled ω-2ω intense laser fields (800 and 400 nm, 3.3 × 1014 W/cm2) using three-dimensional coincidence ion momentum imaging. The two-body Coulomb explosion pathway, CH3CN2+→CH3++CN+, exhibits a clear phase-dependent fragment asymmetry along the laser polarization direction, showing that the tunnel ionization preferentially prepares the acetonitrile dication with the methyl group pointing toward the smaller amplitude side of the laser electric field. The Coulomb explosion pathway occurring after the migration of a single hydrogen atom, CH3CN2+→CH2++HCN+, shows a pronounced reduction in the fragment asymmetry. A clear deuteration effect observed for the asymmetry of the hydrogen-migration pathway suggests that the two-color asymmetric laser field has a significant impact on the directionality of intramolecular hydrogen migration in acetonitrile dication.