Abstract

Nuclear magnetic resonance (NMR) is a central method for investigating the microscopic structure and dynamics of molecules and materials, with numerous applications in science, technology, and medicine. Computational modelling is indispensable in NMR research due to the indirect nature of NMR information and the rich physical phenomenology behind its observables. While NMR is conventionally used to study diamagnetic systems, paramagnetic NMR (pNMR) of electronically open-shell systems is rapidly gaining importance. This inaugural article concerns the methodology and application of computational molecular science to the observables pNMR, including current challenges and outlook for the future.