Abstract
It is shown that large nuclear polarizations in isolated molecules may be created via the hyperfine interaction following excitation to selected rotational states |JM>. Explicit time-dependent nuclear polarization expressions for pulsed rotational excitation are presented for the case of one nuclear spin I, and for the case of two nuclear spins I1 and I2 in the hierarchical coupling limit. Photodissociation of the polarized molecules allows the production of polarized atoms, on short time scales if pulsed, at densities close to the parent molecule density.
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