Yingsheng Wang, Peipei Dang, Zixun Zeng, Dongjie Liu, Guodong Zhang, Long Tian, Kai Li, P. Ma, Yi Wei, Hongzhou Lian, Zhiyao Hou, Guogang Li, Jun Lin
Abstract Lead-free halide double perovskites (LFHDPs) have gained prominence as eco-friendly optoelectronic materials due to their structural stability and flexible tunability. Lanthanide (Ln 3+ ) ions have rich energy levels, which can endow LFHDP materials with emissions ranging from visible to near-infrared (NIR) region through the ion doping strategy. However, their NIR applications remain limited by narrowband emission and low photoluminescence quantum yield (PLQY) due to weak absorption cross-section. Herein, Cs 2 NaInCl 6 :Ln 3+ were successfully synthesized, and the problem of low absorption of Ln 3+ ions is effectively solved. Incorporating Mo 4+ /Ag + ions achieves a near-unity PLQY and expands the excitation spectrum across the full visible range and a small part of NIR region (250–850 nm). Mechanism analysis revealed synergistic energy transfer pathways involving self-trapping excitons and intermediate energy states of Mo 4+ ion, enhancing both photon absorption and PLQY. The universal applicability of this approach has been validated across Bi-based and multiple lanthanide ions (Ln: Ho, Er, Tm, Yb). These optimized materials demonstrate exceptional broadband emission characteristics suitable for multi-scenario NIR applications, including light-emitting-diodes (LEDs), night vision, imaging, anti-counterfeiting technologies. This co-doping methodology establishes a versatile framework for overcoming inherent limitations in Ln 3+ -activated materials, offering new possibilities for efficient NIR optoelectronic devices.