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Quantitative composition‐structure‐property (C–S–P) relationship analysis is a promising approach to correlate structural features with properties of glasses that have complex structures and lack long‐range order. In this study, the structure and spectroscopic properties of two typical P2O5‐MO‐K2O‐Al2O3 (M = Mg, Ba) quaternary phosphate laser glasses doped with Nd3+ ions are calculated and predicted...