Beyond isotropic reorientation: probing anisotropic and internal motions in ionic liquids with fast field cycling NMR relaxometry and MD simulations

groups. For both ILs, self-diffusion coefficients were also obtained in addition to rotational dynamics. Notably, the analysis explicitly considered heteronuclear intermolecular contributions, which were found to play a significant role in accurately capturing the relaxation behavior. Complementary MD simulations provided rotational correlation times and self-diffusion coefficients, which showed excellent agreement with experimental results, thereby validating the employed relaxation models. These findings contribute to a deeper understanding of IL dynamics, emphasizing the role of ion geometry and internal motions in data evaluation. Thereby, this work establishes a comprehensive framework for future studies on complex IL systems.