Characterization by single-crystal X-ray diffraction (XRD) reveals that the unit cell of the obtained structure contains a single pseudo-tetrahedral Ga motif, consisting of Ga bound to 3 siloxide ligands (Ga-O(Si): 1.782-1.794 Å), with the pyridinic-N found in an axial position (Ga-N: 2.008 Å). The O-Ga-O (θO-Ga-O) and O-Ga-N (θO-Ga-L) bond angles fall in the range 110.4-114.0° and 103.7-109.5°, respectively. δiso(15N) of 15 N-1-py (247 ppm, C6D6), is shifted 70 ppm to lower frequency than that of free pyridine, consistent with the interaction of pyridine with Ga. The solid state δiso(15N) (246 ppm), is consistent with the chemical shift assigned to pyridine interacting with a Lewis acidic Ga site in Ga@SiO2 ( 15 N-py/GaLA, δiso(15N) = 236 ppm, vide supra), further supporting the assignment for 15 N-py/GaLA.. The difference in δiso (ca. 10 ppm) found for 15 N-1-py and 15 N-py/GaLA indicates an increased Lewis acidity for the surface species. The increased Lewis acidity of 15 N-py/GaLA vs. 1-py likely arises from increased strain in the surface species Furthermore, fitting of the CSA for the molecular species 15 N-1-py, gives a span (Ω) of 440 ppm, and a skew (κ) of 0.74., which also aligns well with fitting of the CSA for N-py/GaLA (SI S7).