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Title: Spectroscopy, reaction, and photodissociation in highly vibrationally excited molecules. Technical progress report

Technical Report ·
DOI:https://doi.org/10.2172/10134800· OSTI ID:10134800

Highly vibrationally excited molecules often control the course of chemical reactions in the atmosphere, combustion, plasmas, and many other environments. The research described in this Progress Report uses laser excitation and interrogation techniques to study and control the dynamics of highly vibrationally excited molecules. In particular, they show that it is possible to unravel the details and influence the course of photodissociation and bimolecular reaction. The experiments use laser excitation of overtone vibrations to prepare highly vibrationally excited molecules, frequently with single quantum state resolution, and laser spectroscopy to monitor the subsequent behavior of the excited molecule. We have studied the vibrationally mediated photodissociation and the bond- and state-selected bimolecular reaction of highly vibrationally excited molecules. In the first process, one photon creates a highly excited molecule, a second photon from another laser dissociates it, and light from a third laser detects the population of individual product quantum states. This approach allows us to explore otherwise inaccessible regions of the ground and excited state potential energy surface and, by exciting to the proper regions of the surface, to control the breaking of a selected chemical bond. In the second process, the highly vibrationally excited molecule reacts with an atom formed either in a microwave discharge or by photolysis and another laser interrogates the products. We have used this approach to demonstrate mode- and bond-selected bimolecular reactions in which the initial excitation controls the subsequent chemistry. 30 refs., 8 figs.

Research Organization:
Univ. of Wisconsin, Madison, WI (United States)
Sponsoring Organization:
USDOE, Washington, DC (United States)
DOE Contract Number:
FG02-86ER13500
OSTI ID:
10134800
Report Number(s):
DOE/ER/13500-3; ON: DE92010651
Resource Relation:
Other Information: PBD: [1991]
Country of Publication:
United States
Language:
English