Assignment of the He@C84 isomers in experimental NMR spectra using density functional calculations

► The 3He chemical shifts were calculated for Hen@C84 (n = 1, 2) fullerenes. ► Accuracy within 1 ppm could be reached using DFT methods. ► Additional criteria in the interpretation of 3He NMR were discussed. ► Endohedral 3He shifts were predicted for He@C846- anions.