While modelling of the lineshape of the 71 Ga NMR spectrum for CQ species was required to take into account Brønsted acid sites upon deprotonation. In these cases, the lower observed CQ value compared to DFT calculations for the BAS has been ascribed to residual dynamics, consistent with what is observed in GaBA. For the larger CQ species, assigned to ( 15 N-py)/GaLA (𝐶 1 𝑄,0 = 22 MHz), the magnitude of CQ matches well the experimentally obtained value of the corresponding molecular structure Ga(OSi(OtBu)3)3(py) (CQ = 24 MHz), indicating that ( 15 N-py)/GaLA can be described as a Ga motif with three anionic siloxide ligands and one N-bound pyridine. CQ species was required to take into account Brønsted acid sites upon deprotonation. In these cases, the lower observed CQ value compared to DFT calculations for the BAS has been ascribed to residual dynamics, consistent with what is observed in GaBA. For the larger CQ species, assigned to ( 15 N-py)/GaLA (𝐶 1 𝑄,0 = 22 MHz), the magnitude of CQ matches well the experimentally obtained value of the corresponding molecular structure Ga(OSi(OtBu)3)3(py) (CQ = 24 MHz), indicating that ( 15 N-py)/GaLA can be described as a Ga motif with three anionic siloxide ligands and one N-bound pyridine.