Three-Body Dissociation Dynamics of the Low-Lying Rydberg States ofH3andD3

Abstract

The dynamics of the three-body dissociative charge exchange of fast (12 keV) H+3 and D+3 with Cs have been studied using multiparticle translational spectroscopy. The observed partitioning of product momenta was found to be state-specific and yields insights into the nuclear motion during dissociation for the three lowest-lying 2s 2A'1, 2p 2A''2, and 3p 2E' metastable Rydberg states of H3 and the 2s 2A'1 and 2p 2A''2 states for D3. These results provide direct empirical information on the nonadiabatic couplings that govern the three-body dissociation of the lowest-lying Rydberg states of H3 and D3.

Momentum vector correlations in three-particle fragmentation of triatomic hydrogen

“…Clearly, the electronic state scrutinized here is among the most simple situations encountered in triatomic hydrogen. We know from previous studies [4][5][6] that the vector correlation maps show increasing complexity for the higher lying Rydberg states. Further development of semiclassical and quantum simulations of the dissociation process promises more guidance in this regard.…”

“…Multidimensional imaging and coincidence techniques allow us to tackle the three-body dissociation problem experimentally, providing information about correlation in fragment momentum vectors [3][4][5][6]. The basic experimental setup used in Freiburg for neutral triatomic hydrogen is shown Fig.…”

Formation of fragment momentum correlations in three-body predissociation of triatomic hydrogen: The interplay of geometry-dependent nonadiabatic coupling and ground-state dynamics

“…Predissociation of H 3 Rydberg states has attracted much interest over the past two decades [1][2][3][4][5][6][7][8][9][10][11][12]. There are two major reasons for the persistent attention to this subject.…”

“…Recent experimental observations indicate that the effects of such geometric properties are reflected in correlations among the momenta of the three H atoms emerging from threebody predissociation of state-selected H 3 [3,4,12,23]. The states of which three-body predissociation were investigated to date comprise several rovibrational levels of electronic states of H 3 as well as D 3 , especially 2sA 1 , 2pA 2 , 3pE , 3sA 1 , and 3dE .…”

Stark Field Control of Nonadiabatic Dynamics in Triatomic Hydrogen

“…In polyatomic systems the larger number of degrees of freedom complicates the observation and description of dynamical properties [2]. During the last decade powerful experimental techniques have been brought to bear on nonadiabatic processes: Ultrafast lasers make it possible to follow the course of a chemical reaction [3][4][5], molecular beam technology allows the quantum state preparation of reactants as well as the state selective detection of products [6][7][8], and novel multidimensional coincidence measurements provide hitherto inaccessible information about vector correlations in molecular dynamics [9][10][11][12].…”