The challenge of developing phosphors with tailored near-infrared (NIR) emission ranges to meet the diverse demands of various applications is a paramount concern in the contemporary realm of NIR phosphor research. A strong dependence of NIR emission on Cr3+ concentration has been demonstrated in Sc2−xSi2O7:xCr3+, which exhibits an NIR emission band at 840 nm for low Cr3+ doping concentrations (x = 0.001–0.01) and an anomalous NIR emission band at 1300 nm for high Cr3+ doping concentrations (x = 0.01–0.10). Careful investigation of the crystal structure, excitation and emission spectra, and luminescence decay curves indicates that the two NIR emissions can be attributed to the isolated Cr3+ ions and the Cr3+–Cr3+ pairs, respectively. The strong interaction of exchange-coupled Cr3+–Cr3+ pairs is supported by temperature-dependent emission spectra, luminescence decay curves and electron paramagnetic resonance (EPR) measurements. This work provides a new insight into the study of Cr3+–Cr3+ pairs for broadband NIR emission.
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