Importance of Nuclear Quantum Effects for NMR Crystallography

The resolving power of solid-state nuclear magnetic resonance (NMR) crystallography depends heavily on the accuracy computational predictions NMR chemical shieldings candidate structures, which are usually taken to be local minima in potential energy. To test limits this approximation, we systematically study importance finite-temperature and quantum fluctuations for 1H, 13C, 15N polymorphs three paradigmatic molecular crystals: benzene, glycine, succinic acid. effect is comparable typical errors shielding static nuclei with respect experiments, their inclusion improves agreement measurements, translating more reliable assignment spectra correct structure. use integrated machine-learning models, trained first-principles energies shieldings, renders rigorous sampling affordable, setting a new standard calculations underlying structure determinations.