Rational Design of Nd ³ ⁺ ‐Doped Quaternary Silicate Laser Glass via the Phase Diagram Approach

ABSTRACT Establishing the composition–structure–property (C–S–P) relationship in laser glasses is crucial for accelerating their rational design and moving beyond traditional “trial‐and‐error methods.” However, the intrinsic disorder of glass and the complex local environment of rare‐earth ions present significant challenges for predicting spectroscopic properties using existing physical and statistical models. This study focuses on Nd 3+ ‐doped SiO 2 –CaO–Li 2 O–Al 2 O 3 (SCLA) quaternary silicate laser glasses. By employing nearest‐neighboring congruently melting compounds (CMCs) as “structural motifs” and verifying structural correlations via molecular dynamics simulations, we achieve quantitative prediction of key glass properties. For Nd 3+ ‐doped SCLA glasses, the prediction errors for structural parameters and physical properties are less than 5%, while those for spectroscopic parameters are all below 10%. Furthermore, a comprehensive C–S–P database for Nd 3+ ‐doped SCLA laser glasses has been established, including five physical and nine spectroscopic properties across 7800 compositions. This provides reliable data support for the rapid screening and optimization of high‐performance glass compositions. These findings verify the reliability of the phase diagram approach (PDA) for quantitatively predicting spectroscopic properties in complex quaternary systems and offer a promising approach for tailoring the performance of laser glasses.