Kinematically complete final state investigations of molecular photodissociation: two- and three-body decay of laser-prepared H3 3s 2A'1
Fakultät für Physik, Albert-Ludwigs-Universität Freiburg, Hermann-Herder-Strasse 3, 79104 Freiburg, Germany
Corresponding author: a Ulrich.Mueller@uni-freiburg.de
Published online: 15 December 2001
We have performed kinematically complete investigations of molecular photodissociation of triatomic hydrogen in a fast beam translational spectrometer recently built in Freiburg. The apparatus allows us to investigate laser-induced dissociation of neutral molecules into two, three, or more neutral products. The fragments are detected in coincidence and their vectorial momenta in the center-of-mass frame are determined. We demonstrate the potential of the method at the fragmentation of the 3 state of triatomic hydrogen. In this state, three-body decay into ground state hydrogen atoms H+H+H, two-body predissociation into H+(v, J), and photoemission to the ground state surface with subsequent two-body decay are competing channels. In the case of two-body predissociation, we determine the rovibrational population in the (v, J) fragment. The vibrational distribution of is compared with approximate theoretical predictions. For three-body decay, we measure the six-fold differential photodissociation cross-section. To determine accurate final state distributions, the geometric collection efficiency of the apparatus is calculated by a Monte Carlo simulation, and the raw data are corrected for apparatus efficiency. The final state momentum distribution shows pronounced correlation patterns which are characteristic for the dissociation mechanism. For a three-body decay process with a discrete kinetic energy release we have developed a novel data reduction procedure based on the detection of two fragments. The final state distribution determined by this independent method agrees extremely well with that observed in the triple-coincidence data. In addition, this method allows us to fully explore the phase space of the final state and to determine the branching ratios between the two- and three-body decay processes.
PACS: 33.80.Gj – Diffuse spectra; predissociation, photodissociation / 33.80.Rv – Multiphoton ionization and excitation to highly excited states (e.g., Rydberg states) / 34.80.Ht – Dissociation and dissociative attachment by electron impact
© EDP Sciences, Società Italiana di Fisica, Springer-Verlag, 2001