The rovibrational state distributions of both the CS and the SO products fo
llowing the reaction of O(P-3) + CS2 have been investigated. The O(P-3) ato
ms are generated by photolysis of NO:! using a frequency-tripled Nd:YAG las
er at 355 nm. The SO(X(3)Sigma (-), upsilon" = 0-6) and CS(X(1)Sigma (+), u
psilon" = 0-3) are observed directly using laser induced fluorescence (LIF)
spectroscopy on the (B(3)Sigma (-) - X(3)Sigma (-)) and (A(1)II - X(1)Sigm
a (+)) transitions, respectively. The SO(X(3)Sigma (-)) product is found to
be highly excited with the vibrational state distribution inverted at upsi
lon" = 1 and detectable population up to upsilon" = 6, while the CS(X(1)Sig
ma (+)) product vibrational state distribution is characterized as Boltzman
n with a vibrational temperature of 1230 +/- 155 K. The total vibrational e
xcitation of both products accounts for 21% of the available energy to the
products. The near nascent SO(X(3)Sigma (-), upsilon" 0-4) rotational state
distributions are characterized by rotational temperatures in the range of
882-1312 K, and the near nascent CS(X(3)Sigma (+), upsilon" = 0) is charac
terized by a temperature of 2986 +/- 607 K. The total rotational energy of
the products accounts for 34.8% of the available energy. Correlated ah init
io calculations of the reaction pathway have been performed, resulting in a
ccurate energies for the reactants, products, intermediates, and transition
states. Optimized geometries for the intermediates and transition states h
ave been obtained. The inverted vibrational state distribution of the SO(X(
3)Sigma (-)) product and the excited rotational state distribution of the C
S(X(1)Sigma (+)) product suggest a short-lived, nonlinear intermediate stru
cture as the primary pathway for the reaction. The results from the ab init
io calculations corroborate this model.