A two-dimensional (2D) experiment has been used to show that 14N irradiation and magic-angle spinning (MAS) results in population transfers between the 14N Zeeman levels. This experiment was applied to a sample of N-acetyl-D,L-valine, a material where asymmetric doublets resulting from 13C-14N dipolar coupling are clearly resolved in the 13C spectrum at a field of 7 T for Carbon atoms directly bonded to the nitrogen atom. The 13C transverse magnetization was allowed to evolve in the F1 and F2 dimensions, and the 14N spins were irradiated during the mixing period. Cross-peaks were observed in the 2D 13C spectrum between the two peaks of the CH asymmetric doublet. Since one peak of the doublet results primarily from coupling to the [formula: see text] state and the other peak from coupling to [formula: see text] states, population changes between the 14N Zeeman levels have occurred during the mixing period. These population transfers are a consequence of the time dependence of the 14N quadrupole splitting Q under MAS conditions and 14N irradiation. Level anti-crossings of the 14N Zeeman levels occur at the zero-crossings of Q, and a continuous and slow change in Q will result in the transfer of 14N populations between the different Zeeman levels. If these passages are adiabatic, then the system returns to its original state after two zero-crossings. This is consistent with the experimental observation that the intensities of the cross-peaks for 14N irradiation are greater for half a rotor period than a full rotor period.