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<p>Hot carriers, inheriting excess kinetic energy from high-energy photons, drive numerous optoelectronic applications reliant on non-equilibrium transport processes. Although extensively studied in inorganic materials, their potential in organic-based systems remains largely unexplored. Here we demonstrate highly mobile hot carriers in crystalline two-dimensional conjugated coordination polymer Cu<sub>3</sub>BHT (BHT, benzenehexathiol) films. Leveraging a suite of ultrafast spectroscopic and imaging techniques, we map the microscopic charge transport landscape in Cu<sub>3</sub>BHT films following non-equilibrium photoexcitation across temporal, spatial and frequency domains, revealing two distinct high-mobility transport regimes. In the non-equilibrium regime, hot carriers achieve an ultrahigh mobility of ~2,000 cm<sup>2</sup> V<sup>–1</sup> s<sup>–1</sup>, traversing grain boundaries up to ~300 nm within a picosecond. In the quasi-equilibrium regime, free carriers exhibit Drude-type, band-like transport with a remarkable mobility of ~400 cm<sup>2</sup> V<sup>–1</sup> s<sup>–1</sup> and an intrinsic diffusion length exceeding 1 μm. These findings position two-dimensional conjugated coordination polymers as versatile platforms for advancing organic-based hot carrier applications.</p>

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Unveiling high-mobility hot carriers in a two-dimensional conjugated coordination polymer

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年5月13日

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  • Shuai Fu,
  • Xing Huang,
  • Guoquan Gao,
  • Petko St. Petkov,
  • Wenpei Gao,
  • Jianjun Zhang,
  • Lei Gao,
  • Heng Zhang,
  • Min Liu,
  • Mike Hambsch,
  • Wenjie Zhang,
  • Jiaxu Zhang,
  • Keming Li,
  • Ute Kaiser,
  • Stuart S. P. Parkin,
  • Stefan C. B. Mannsfeld,
  • Tong Zhu,
  • Hai I. Wang,
  • Zhiyong Wang,
  • Renhao Dong,
  • Xinliang Feng,
  • Mischa Bonn

摘要

Hot carriers, inheriting excess kinetic energy from high-energy photons, drive numerous optoelectronic applications reliant on non-equilibrium transport processes. Although extensively studied in inorganic materials, their potential in organic-based systems remains largely unexplored. Here we demonstrate highly mobile hot carriers in crystalline two-dimensional conjugated coordination polymer Cu3BHT (BHT, benzenehexathiol) films. Leveraging a suite of ultrafast spectroscopic and imaging techniques, we map the microscopic charge transport landscape in Cu3BHT films following non-equilibrium photoexcitation across temporal, spatial and frequency domains, revealing two distinct high-mobility transport regimes. In the non-equilibrium regime, hot carriers achieve an ultrahigh mobility of ~2,000 cm2 V–1 s–1, traversing grain boundaries up to ~300 nm within a picosecond. In the quasi-equilibrium regime, free carriers exhibit Drude-type, band-like transport with a remarkable mobility of ~400 cm2 V–1 s–1 and an intrinsic diffusion length exceeding 1 μm. These findings position two-dimensional conjugated coordination polymers as versatile platforms for advancing organic-based hot carrier applications.