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Momentum correlations in three-body predissociation of triatomic hydrogen are investigated by quasiclassical trajectory calculations. It is shown that nonadiabatic couplings that trigger predissociation of the 2sA 1 state of H 3 imprint their geometric properties on the momentum correlation structures observed after dissociation. A simple symmetry-based model of the geometric coupling properties succeeds in reproducing most of the experimentally observed patterns. The ground-state dynamics that transform the geometric properties of the coupling into the final momentum correlations are identified.

We show in an experiment that dissociation of state-selected neutral H3* molecules into three ground-state hydrogen atoms reveals highly structured maps of correlation in the motion of the three atoms. These maps provide a direct view of the internal molecular couplings which initiate dissociation.

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The correlation pattern in the center of mass motion of the three fragments from dissociation of well-defined Rydberg states of H 3 and D 3 is studied. Dissociation of the molecules is induced by an external electric field. Through a comparison with results obtained in radiative cascading we can show that the correlation pattern is that of the short-lived 2s 2 A 1 electronic state, of which a tiny amplitude is admixed by the external electric field. A comparison of our results with the predictions by M. Lehner and M. Jungen [J. Phys. B 42, 065101 (2009)] and U. Galster [Phys. Rev. A 81, 032517 (2010)] for predissociation of the 2s 2 A 1 state is made. We show that the experimental vector correlation maps are direct images of the spatial symmetry of the product of the vibrational wave function and spatial dependence of the nonadiabatic coupling operator.

We determine experimentally the vector correlation among the three neutral ground state hydrogen atoms which appear in dissociation of neutral H3* molecules. The sum of the kinetic energies of the three H-atoms is fixed by selecting the energy of the H3* molecule by laser excitation in the range between 0.85 and 3.60 eV. The highly structured maps of correlation in the motion of the three atoms provide a direct view of the internal molecular couplings which initiate dissociation. We discuss this feature in a model calculation and in terms of a new quantum chemical calculations of the potential energy surfaces of H3*.

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