One possible explanation for the deviation between the calculated and experimental results relates to disorder on the lithium site. Lithium coordination in LiIn 2 SbO 6 was previously probed by Li and Li NMR where it was determined that the unique tunnel pattern of this rutile-like structure hosts lithium ions in split tetrahedral sites. This finding ran counter to a previous proposal that LiIn 2 SbO 6 is simply a cation-ordered variant of LiSbO 3 with octahedral LiO 6 sites. The Li NMR, however, is unable to resolve the question of whether it is disordered (statically or dynamically) in the split tetrahedral site, which may affect the indium and antimony via next-nearest-neighbor interactions. It is also possible that the computed EFG parameters for In and 121 Sb in LiIn 2 SbO 6 are underestimated, which is a known issue in a variety of systems. Solid-state NMR of BiMTeO 6 (M = Al, Ga). The frequency-stepped VOCS method with QCPMG pulses was also used to record (ultra-)wideline CT and partial ST spectra of BiAlTeO 6 and BiGaTeO 6 covering more than 16 MHz (Figure , Supplementary Figure ).