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Bismuth (Bi)‐doped laser glasses with broadband emission are of current interest in the fields of sensing, bio‐imaging, and photonics. For practical applications, it must be considered how to improve the emission efficiency, in particular, for borate glasses with wide glass‐forming range, low melting point, and excellent fiberizing ability. Herein, we experimentally demonstrate that addition of GeO2 to aluminoborate glasses can effectively enhance Bi NIR emission by more than 300 times with prolonged decay time (~500 μs) and good homogeneity, which is, to our best knowledge, seldom achieved in Bi‐doped borate multi‐component glasses. The addition of second glass‐former GeO2, as revealed by detailed optical and structural analysis, leads to the facile regulation on local glass structure, forcing the conversion of aluminum species from AlO5 and AlO6 to AlO4 and consequently pushes the conversion of Bi3+ to Bi+ and Bi0 and stabilizes Bi NIR centers, which finally results in highly enhanced Bi NIR emission. We believe these results could contribute to designing Bi‐activated multi‐component laser glass and fibers with efficient NIR photoemission. [ABSTRACT FROM AUTHOR]

Abstract: Because of ultra‐broadband near‐infrared (NIR) emission bismuth‐activated glasses and fibers offer a new promising platform for novel photonic devices such as new type of optical amplifiers and broadly tunable fiber lasers. Yet, challenge remains to manipulate the NIR emission behavior of bismuth (Bi) in photonic glasses for efficient Bismuth‐doped fiber and fiber lasers. Here, by engineering phosphorus and aluminum's topology, broadly tunable NIR emission has been realized in Bismuth‐doped phosphate laser glass. Structural and optical analyses on 27Al magic‐angle spinning nuclear magnetic resonance (MAS NMR), 31P MAS NMR, fourier transform infrared (FTIR) and static emission spectra suggest that polymerization of glass network can be improved by proper addition of aluminum into the system, which can be evidenced by partial conversion of Q2 to Q3 species of phosphorus and the shift of P–O–P asymmetric stretching vibration toward lower frequency, and this turns out beneficial to Bi NIR emission. Embedding aluminum tetrahedra into phosphorus glass network can reduce the local crystal field around bismuth and therefore lead to the blueshift of Bi emission. This work presents new insights into the luminescent behavior of Bi ions in phosphate glass and it helps the design and fabrication of Bismuth‐doped glasses and fibers in future. [ABSTRACT FROM AUTHOR]