PHOTODISSOCIATION DYNAMICS OF DOUBLY EXCITED RYDBERG STATES OF MOLECULAR-HYDROGEN

We have applied photofragment ion imaging to investigate the dissociation dynamics of low-lying, doubly excited states of molecular hydrogen. A doubly excited electronic state is one in which both of the hydrogen electrons reside in excited molecular orbitals. Two-step, two-color multiphoton excitat...

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Bibliographic Details
Published in:The Journal of chemical physics 1992-04, Vol.96 (8), p.5843-5856
Main Authors: BUNTINE, MA, BALDWIN, DP, CHANDLER, DW
Format: Article
Language:English
Subjects:
ATOMIC AND MOLECULAR PHYSICS
AUTOIONIZATION
Chemistry
Chemistry, Physical
COLOR
DISSOCIATION
DISTANCE
DYNAMICS
ELEMENTS
ENERGY LEVELS
Exact sciences and technology
EXCITED STATES
HYDROGEN
INTERATOMIC DISTANCES
IONIZATION
MECHANICS
Molecular properties and interactions with photons
MOLECULES
MULTI-PHOTON PROCESSES
NONMETALS
OPTICAL PROPERTIES
ORGANOLEPTIC PROPERTIES
Photon interactions with molecules
PHYSICAL PROPERTIES 664200 > Spectra of Atoms & Molecules & their Interactions with Photons-- (1992-)
Physical Sciences
Physics
Physics, Atomic, Molecular & Chemical
RYDBERG STATES
Science & Technology
VELOCITY
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Summary:We have applied photofragment ion imaging to investigate the dissociation dynamics of low-lying, doubly excited states of molecular hydrogen. A doubly excited electronic state is one in which both of the hydrogen electrons reside in excited molecular orbitals. Two-step, two-color multiphoton excitation of H-2, first via 201.8 nm, two-photon excitation into the E, F (1)SIGMA(g)+ (upsilon(E) = 0, J = 1) state, followed by approximately 563 nm, 1 + m (m = 1, 2) excitation through the B" (1)SIGMA(u)+ (upsilon = 0, J = 0, 2), D (1)PI(u) (upsilon = 2, J = 1, 2), and B' (1)SIGMA(u)+ (upsilon = 4, J = 0, 2) states provides a ready means of populating several low-lying doubly excited states of H-2 at increasing internuclear separations. From these doubly excited repulsive states, both dissociation and autoionization processes are possible. Because the excitation energy remains relatively constant as each intermediate state is accessed, differences in the photodissociation dynamics via each state can be ascribed directly to the effects of changing internuclear separation and electronic symmetry of the intermediate and dissociative states. H+ fragments detected from each photodissociation pathway are distinguished by their differing velocities, determined from an ion image.
ISSN:0021-9606
1089-7690
DOI:10.1063/1.462682