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Direct identification of photofragment structures formed in the 193 nm photodissociation of thiophene

Journal Article · · Journal of Physical Chemistry; (United States)
DOI:https://doi.org/10.1021/j100006a019· OSTI ID:6766697

An experimental scheme which involves vacuum ultraviolet photoionization mass spectrometric sampling of laser photodissociation products in a pulsed supersonic molecular beam has been used to identify the isomeric structures of the 193 nm photofragments from thiophene. The primary products observed are vinylacetylene (H[sub 2]C=CH-C=CH), acetylene (C[sub 2]H[sub 2]), and thioketene (H[sub 2]C=C=S). Using the 2 + 1 resonance-enhanced multiphoton (REMPI) scheme, we find that S atoms are produced predominantly ([ge]96%) in [sup 3]P[sub J] states with a fine structure distribution of [sup 3]P[sub 2]:[sup 3]P[sub 1]:[sup 3]P[sub 0] = 0.82 [+-] 0.03:0.15 [+-] 0.03:0.03 [+-] 0.03. These experimental results indicate that the major dissociation channels are CH[sub 2]=CH-C=CH + S([sup 3]P) and CH=CH + CH[sub 2]=C=S. Ab initio multiconfiguration self-consistent-field calculations have been made to rationalize these experimental observations. 52 refs., 4 figs., 3 tabs.

DOE Contract Number:
W-7405-ENG-82
OSTI ID:
6766697
Journal Information:
Journal of Physical Chemistry; (United States), Journal Name: Journal of Physical Chemistry; (United States) Vol. 99:6; ISSN JPCHAX; ISSN 0022-3654
Country of Publication:
United States
Language:
English