Abstract The time-domain NMR signal that results from chemical shifts or first-order quadrupolar effects in materials with either a few well-defined sites or a distribution in orientation or coupling constants is given by an integral of exp[ikt(3 cos2θ − 1)] or exp[ikt(3 cos2θ − 1 + η sin2θ cos 2 φ)] times a weighting probability for orientation and/or coupling constants. Data analysis requires either execution of angular averages, as for a powder sample, or determination of the weighting function, as for an oriented sample. Development of expansions of the above exponential forms in spherical harmonics for use in such data analysis is initiated. This development is analogous to the Ray leigh expansion of exp (ikr cos θ) in spherical harmonics that is ubiquitous throughout scattering theory. Applications to analysis of a 2D NMR experiment, characterization of anisotropic materials, and determination of the distribution of coupling constants are discussed as examples of the reduction of computation time, by use of analytic, rather than the currently used numerical, execution of angular averages. It is also expected that the availability of algebraic forms provides a useful alternative perspective, complementary to numerical calculations, offering a potential for direct extraction of motional correlation functions from NMR data and estimation of orientation probabilities. A transformation needed for application of the expansion to magic-angle spinning of rigid-lattice samples is developed.
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