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Fragmentation of cyano compounds under nonlinear UV excitation: delayed CN B/sup 2/. sigma. /sup +/ chemiluminescence through ion-molecule collisions

Journal Article · · J. Phys. Chem.; (United States)
DOI:https://doi.org/10.1021/j100285a015· OSTI ID:6800021
UV nonlinear excitation (266 nm, 4.66 eV; 22 ps) of various molecular gases may create small populations distributed over several quantum orders nhv/sub 266/, initiating distinct processes. With subnanosecond time resolution, the authors have distinguished prompt (unimolecular) and delayed (collisional) components of fragment emission in the CN violet bands, from the cyano compounds XCN (X = Cl, CN, and CH/sub 3/). A quantitative kinetic analysis of CN B/sup 2/..sigma../sup +/ ..-->.. X/sup 2/..sigma../sup +/ oscilloscope traces and comparison of the rate constants with AADO/AQO rate theory lead to the inference that the delayed emission arises through ion-molecule collisions. In our preferred picture the ions are identified as long-lived excited states of the parent species XCN/sup +/. Our previous findings with isotopically labeled CH/sub 3/CN, in particular the inference of isomerization, are quite consistent with this hypothesis. The authors suggest that similar ion-molecule channels may give rise to delayed chemiluminescence from a wide variety of simple molecules.
Research Organization:
Naval Research Lab., Washington, DC
OSTI ID:
6800021
Journal Information:
J. Phys. Chem.; (United States), Journal Name: J. Phys. Chem.; (United States) Vol. 91:1; ISSN JPCHA
Country of Publication:
United States
Language:
English