C-REDOR curves of extended spin systems

The convergence of simulated C-REDOR curves of (infinitely) large spin systems is investigated with respect to the number of spins considered in the calculations. Taking a sufficiently large number of spins (>20,000 spins) into account enables the simulation of converged C-REDOR curves over the entire time period and not only the initial regime. The calculations are based on an existing approximation within first order average Hamiltonian theory (AHT), which assumes the absence of homonuclear dipole-dipole interactions. The C-REDOR experiment generates an average Hamiltonian close to the idealized AHT behavior even for multiple spin systems including multiple homonuclear dipole-dipole interactions which is shown from numerically exact calculations of the spin dynamics. Experimentally it is shown that calculations accurately predict the full, experimental C-REDOR curves of the multi-spin systems (31)P-(19)F in apatite, (31)P-(1)H in potassium trimetaphosphimate and (1)H-(31)P in potassium dihydrogen phosphate. We also present (13)C-(1)H and (15)N-(1)H data for the organic compounds glycine, l-alanine and l-histidine hydrochloride monohydrate which require consideration of molecular motion. Furthermore, we investigated the current limits of the method from systematic errors and we suggest a simple way to calculate errors for homogeneous and heterogeneous samples from experimental data.