An experimental method based on the technique of microwave pumping was used to measure spin-phonon transition probabilities in dilute potassium chromi-cyanide. The set of numerical values obtained appears to indicate that the spin-lattice relaxation by the direct process of the cyanide-coordinated Cr3+ ion violates the quadrupolar selection rules. This behavior is in disagreement with the Kronig – Van Vleck theory, but is not contradicted by the experimental results of other workers.