“…Further, in terms of mixing/de-mixing of network-forming moieties with the introduction of Ca 2+ to the investigated glass systems, though it is challenging to zero down on the exact reason for the trends observed in D-HMQC NMR studies, based on the results of 1D MAS NMR spectroscopy, MD simulations, and literature [81][82][83], it can be hypothesized that the following structural descriptors play an essential role in dictating the observed trends: (1) Na/Al and R; (2) the ionic field strength of Ca 2+ ; (3) which cation -Na + or Ca 2+ -is charge-compensating AlO 4 − units. The abovementioned structural descriptors will be instrumental in deciding the (1) short-range ordering in the glass structure, i.e., silicate, borate, and aluminate speciation, (2) concentration and stabilization of Al-O-Al linkages [68], (3) concentration of ring/non-ring BO 3 units and their connectivity with SiO 4 or BO 4 units [75], and (4) chemical environment around the aluminosilicate network, thus, defining the mixing/de-mixing of network forming units in the glass structure.…”