Abstract
In this review, the process of extracting precise values for NMR interaction tensors from single crystal samples is systematically explored. Starting with a description of the orientation dependence of the considered interactions, i.e., chemical shift, dipolar, and quadrupole interaction, the techniques for acquiring and analysing single-crystal spectra are outlined. This includes the 'classical' approach, which requires the acquisition of three rotation patterns around three rotation axes that are orthogonal to each other, as well as more recent strategies aimed at reducing the number of required NMR spectra. One such strategy is the 'single-rotation method', which exploits the symmetry relations between tensors in the crystal structure to reduce the necessary amount of orientation-dependent data. This concept may be extended to additionally include the orientation of the goniometer axis itself in the data fit, which may be termed the 'minimal-rotation method'. Other, more exotic schemes, such as the use of specialised probe designs or the investigation of single crystals under magic-angle-spinning, are also briefly discussed. Actual values of NMR interaction tensors as determined from the various single-crystal methods have been collected and are provided in tables for spin I=1/2, I=1, and half-integer spins with I>1/2.