Noble Metals Doping in Lead-Free Double Perovskite Single Crystals: Achieving Near-Infrared to X-ray Broadband Photodetection

无铅双钙钛矿单晶中的贵金属掺杂:实现近红外到X射线宽带光电探测

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Abstract

Semiconductor materials capable of broadband photodetection, spanning X-rays to near-infrared (NIR), are essential for applications in medical imaging, industrial inspection, security, and telecommunications. Conventional photodetectors like Si, Ge, InGaAs, and amorphous Se (a-Se) often encounter tradeoffs in efficiency or cost-effectiveness. Halide perovskites (HPs) offer competitive or superior optoelectronic properties with low-cost, solution-based processing. However, lead-based HPs pose toxicity and stability challenges, while lead-free tin-based HPs suffer from Sn(2+) oxidation and structural degradation. The lead-free double perovskite Cs(2)AgBiBr(6) has emerged as a stable, nontoxic alternative for X-ray and visible-light photodetection. Despite its advantages, its high bandgap (≈1.9 eV) limits NIR absorption. This study explores doping Cs(2)AgBiBr(6) with noble metal cations (Au(3+), Pd(2+), and Ir(3+)) to lower its absorption onset and enhance its photodetection capabilities across a broad spectrum. The results demonstrate that noble metal doping can overcome the intrinsic limitations of pristine Cs(2)AgBiBr(6), enabling efficient photodetection from X-rays to the NIR range. This approach highlights a viable pathway for developing next-generation broadband photodetectors that combine nontoxicity, stability, and wide-spectrum sensitivity.

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