Nmr On Single Crystals Of Potassium Cyanogen Bromide (A Measurement Of The Orientational Probability Distribution Function Of The Negatively Charged Cyanogen Ion)

Single crystals of K(CN)$\sb{\rm x}$/(Br)$\sb{\rm 1-x}$ enriched in $\sp{15}$N have been studied by $\sp{15}$N NMR. Because of the anisotropic chemical shift, the NMR frequency spectrum of the orientational glass state reflects the distribution of cyanide orientations. By studying the spectrum at many orientations of each crystal, the orientational probability distribution function P($\Omega$) has been determined for x = 0.50 and for x = 0.20. The probability function is largest along the (100) directions, intermediate in the (110) directions, and nearly 0 along the (111) directions. The NMR determined P($\Omega$) is presented graphically and in terms of the Kubic Harmonic functions. The NMR results are in sharp contrast to molecular dynamics calculations but agree with neutron scattering data for x = 0.53.