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In this work, the relationship among the thermal history, refractive index (RI), and structures of Yb3+/Al3+/P5+/F−‐co‐doped silica glass is studied. We reveal the structural origin of the thermally induced RI change in the Heraeus F300 and Yb3+/Al3+/P5+/F−‐co‐doped silica glasses with different states of thermal history by advanced solid‐state nuclear magnetic resonance and Raman scattering techniques,...