An emerging paradigm in theoretical molecular and materials sciences is computational spectroscopy, which in the case of magnetic resonance spectroscopy means computing directly the primary experimental observables, the time-dependent magnetization or the resulting spectrum. This is to be compared with the traditional way in which comparison with experiment is done at the level of NMR spectral parameters or relaxation times, which themselves result from applying theoretical models to the measurement data. We realise computational spectroscopy by multiscale modelling of atomic dynamics within the material; electronic interactions of the spins at each set of atomic positions and the resulting time dependence of the n
