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<p>Tin–lead (Sn–Pb) halide perovskite single crystals combine narrow bandgaps, long carrier diffusion lengths, and low trap densities, positioning them as ideal candidates for near-infrared (NIR) optoelectronics. However, conventional growth strategies rely on bulk crystallization at elevated temperatures, leading to uncontrolled nucleation, Sn<sup>2+</sup> oxidation, and poor compatibility with planar integration. Here, we develop a coordination-engineered crystallization strategy that enables direct, low-temperature growth of micrometer-thick Sn–Pb single-crystal thin films on device-compatible substrates. By modulating metal–solvent coordination strength using a low-donor number cosolvent system, we delineate a narrow processing window that stabilizes precursor speciation, lowers the nucleation barrier, and guides directional crystal growth under mild thermal conditions (&lt; 40&#xa0;°C). The resulting crystal films exhibit smooth morphology, high crystallinity, compositional uniformity, and ultralow trap densities (~ 3.98 × 10<sup>12</sup>&#xa0;cm<sup>−3</sup>). When integrated into NIR photodetectors, these films deliver high responsivity (0.51 A W<sup>−1</sup> at 900&#xa0;nm), specific detectivity up to 3.6 × 10<sup>12</sup> Jones, fast response (~ 188&#xa0;μs), and &gt; 25,000 cycles of ambient operational stability. This approach establishes a scalable platform for redox-stable, low-temperature growth of Sn–Pb perovskite crystal films and expands the processing–structure–function landscape for next-generation infrared optoelectronics.</p><p></p>

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Monolithic Integration of Redox-Stable Sn–Pb Halide Perovskite Single-Crystalline Films for Durable Near-Infrared Photodetection

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月12日

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  • Rajendra Kumar Gunasekaran,
  • Jihoon Nam,
  • Myeong-geun Choi,
  • Won Chang Choi,
  • Sunwoo Kim,
  • Doyun Im,
  • Yeonghun Yun,
  • Yun Hwa Hong,
  • Sang Hyeok Ryou,
  • Hyungwoo Lee,
  • Kwang Heo,
  • Sangwook Lee

摘要

Tin–lead (Sn–Pb) halide perovskite single crystals combine narrow bandgaps, long carrier diffusion lengths, and low trap densities, positioning them as ideal candidates for near-infrared (NIR) optoelectronics. However, conventional growth strategies rely on bulk crystallization at elevated temperatures, leading to uncontrolled nucleation, Sn2+ oxidation, and poor compatibility with planar integration. Here, we develop a coordination-engineered crystallization strategy that enables direct, low-temperature growth of micrometer-thick Sn–Pb single-crystal thin films on device-compatible substrates. By modulating metal–solvent coordination strength using a low-donor number cosolvent system, we delineate a narrow processing window that stabilizes precursor speciation, lowers the nucleation barrier, and guides directional crystal growth under mild thermal conditions (< 40 °C). The resulting crystal films exhibit smooth morphology, high crystallinity, compositional uniformity, and ultralow trap densities (~ 3.98 × 1012 cm−3). When integrated into NIR photodetectors, these films deliver high responsivity (0.51 A W−1 at 900 nm), specific detectivity up to 3.6 × 1012 Jones, fast response (~ 188 μs), and > 25,000 cycles of ambient operational stability. This approach establishes a scalable platform for redox-stable, low-temperature growth of Sn–Pb perovskite crystal films and expands the processing–structure–function landscape for next-generation infrared optoelectronics.