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By Edwin S. Crawley, Henry B. Evans

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This was used to help characterise the nature of the excited electronic parent molecular states and provide information on the topography of the potential surfaces over which the predissociation proceeds. The photofragment fluorescence excitation spectra from HCN and DCN are displayed in Figs. 8; all the major vibronic bands can be attributed to progressions in the C IA' state, and the CN(B ~ X) fluorescence is polarized positively, confirming the A' symmetry in the upper state 177). The absence of any progressions which involve excitation of the C - H stretching mode vl' in HCN contrasts with the structure observed in the corresponding spectrum for DCN, where progressions with v[' ~< 2 are quite sharp and spectral line broadening only becomes pronounced when v]' = 3 (see Fig.

2 summarises the energetics o f alternative primary processes at shorter wavelengths). In many of the earlier studies 217) a variable deficiency o f 02 was observed in the dissociation products compared with the expected stoichiometric ratio 02 :CO = 0,5 but more recent work has established that the discrepancy is apparent rather than real, and is caused by secondary heterogeneous reactions on the vessel wall 21a). 25 over the range A (174--210) nm 219). At wavelengths 2~< 167 nm, O(1D) becomes energetically accessible [reaction(ii)].

2 nm. /nm Fig. 6. , Ref. 227)) 47 M. N. R. Ashfold, M. T. Macpherson,and J. P. Simons 10 C02 CO+0 ,J'A" lIlg/~ 0 A' ,_ _ 6 (X~. r x Iii // / A' 1 O 12~ A' Fig. 7. Adiabatic singlet electronic state correlation diagram for CO2 dissociation The specificity of the dissociation path leading to O(]S) is easily understood on the basis of a minimum symmetry correlation diagram; similarly for O(IS) from N20, S(1S) from OCS and Se(iS) from OCSe (see later discussion). 7 shows the correlations in the singlet manifold for CO2 and it is clear that it is exclusively the lowest 1l~u + ([A') state which correlates adiabatically with CO( 12;+) + O(1S).

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