Therefore, we propose a comprehensive approach that is able to capture dynamic effects across multiple chemical exchange regimes (Fig. ). By sampling rare events with both MD and transition state searching we obtain effective isotropic and anisotropic O NMR tensors and lineshape simulations. To facilitate accurate sampling and the calculation of transitions states we train a ML force field to near ab-initio accuracy. The MLFF training follows the active learning approach detailed in Reference [74]. These methods allows us to deconvolute the multi-layered dynamics in the example case of MFU-4l MOF: