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Ultraviolet photodissociation of SH (X 2Pi, upsilon"=2-7) and SD (X 2Pi, upsilon"=3-7) has been studied at 288 and 291 nm, using the velocity map imaging technique to probe the angular and speed distributions of the S(1D2) products. Photodissociation cross sections for the A 2Sigma+<--X 2Pi(upsilon") and 2Delta<--X 2Pi(upsilon") transitions have been obtained by ab initio calculations at the CASSCF-MRSDCI/aug-cc-pV5Z level of theory. Both the experimental and theoretical results show that SH/SD photodissociation from X 2Pi (upsilon"<or=7) proceeds via the repulsive wall of the A 2Sigma+ state. The angular distributions of S(1D2) indicate that the dissociation approaches the sudden recoil limit of the A 2Sigma+ state, yielding strongly polarized fragments. The S(1D2) atoms are predominantly produced with total electronic angular momentum perpendicular to the recoil axis.

Photodissociation of vibrationally excited SH and SD radicals at 288 and 291nm: The S(D21) channel