The frequency dependence of the spin-lattice relaxation time T1 was measured at three temperatures near one of the Zeeman-tunneling level matching resonances for pentamethylbenzene. These measurements are correlated with T1 temperature dependence data from the literature. It is shown that the frequency dependence of the Zeeman-torsion coupling time cannot be explained in terms of the semiclassical perturbation theory using time correlation functions. A three bath polarization transfer model is also employed and the applicability of both models discussed. Zeeman-torsion coupling is further investigated using a saturation sequence and the results are compared with the predictions of the three bath polarization transfer model. © 1985, Walter de Gruyter. All rights reserved.