Decay of highly correlated spin states in a dipolar-coupled solid: NMR study of CaF2

We have measured the decay of NMR multiple quantum coherence intensities both under the internal dipolar Hamiltonian as well as when this interaction is effectively averaged to zero, in the cubic calcium fluoride CaF2 spin system and the pseudo-one-dimensional system of fluoroapatite. In calcium fluoride the decay rates depend both on the number of correlated spins in the cluster, as well as on the coherence number. For smaller clusters, the decays depend strongly on coherence number, but this dependence weakens as the size of the cluster increases. The same scaling was observed when the coherence distribution was measured in both the usual Zeeman or z basis and the x basis. The coherence decay in the one-dimensional fluoroapatite system did not change significantly as a function of the multiple quantum growth time, in contrast to the calcium fluoride case. While the growth of coherence orders is severely restricted in this case, the number of correlated spins should continue to grow, albeit more slowly. All coherence intensities were observed to decay as Gaussian functions in time. In all cases the standard deviation of the observed decay appeared to scale linearly with coherence number.