Quasiclassical trajectory calculations with model potential energy surfaces have been used to elucidate the formation dynamics of open-shell radical clusters by “gentle-recoil” photolysis of closed-shell hydride clusters. Specifically, model surfaces for Ar–H2S and Ar2–H2S have been constructed and used to explore photofragmentation dynamics at 193 and 248 nm for comparison with previous experimental results. A remarkable efficiency (as high as 25%) for forming highly excited radical Ar–SH and Ar2–SH clusters is calculated, despite photolysis recoil energies more than 100-fold in excess of the dissociation limit. This surprisingly high survival probability is traced to two dynamical sources. First, ejection of the light H atom from Arn–H2S effectively removes all but a small fraction of the excess photolysis energy from the nascent radical cluster in the center-of-mass frame. Second, although trajectory calculations indicate that nearly 50% of the surviving clusters contain energies up to two-fold higher than the dissociation limit, these clusters are classically bound due to novel angular momentum barriers predicted by Pollak [J. Chem. Phys. 86, 1645 (1987)] for a polyatomic system. Finally, an analysis is presented that indicates the “gentle-recoil” photolysis mechanism may permit efficient formation of highly internally excited, chemically reactive radical clusters of OH and SH with light species such as H2 and D2.