The theory of spin exchange between optically pumped alkali-Inetal atoms and noble-gas nuclei is presented. Spin exchange with heavy noble gases is dominated by interactions in long-lived van der Waals molecules. The main spin interactions are assumed to be the spin-rotation interactions yN S between the rotational angular momentum N of the alkali-metalnoble-gas pair and the electron spin S of the alkali-metal atom, and the contact hyperfine interaction aK S between the nuclear spin K of the noble-gas atom and the electron spin S. Arbitrary values for EC and for the nuclear spin I of the alkali-metal atom are assumed. Precise formal expressions for spin transfer coefficients are given along with convenient approximations based on a perturbation expansion in powers of (o. '/yX), a quantity which has been shown to be small by experiment.

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