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<p>While organic semiconductors (OSCs) offer potential for next-generation electronics, <i>n</i>-type doping in solution-processed OSCs consistently lags behind <i>p</i>-type doping in efficiency, stability, and reproducibility. A fundamental limitation is the lack of a comprehensive understanding of specific molecular interactions between OSCs and dopants at the structural level. This study addresses this challenge by investigating leuco-Rhodamine B (leuco-RhoB) as an <i>n</i>-type dopant for two polymer OSCs of DPP-DTT and N2200. Combining experimental methods with density functional theory calculations, we elucidate the molecular interactions governing OSC-dopant binding preferences and their impact on electrical performance. Spatial overlap between the van der Waals volumes of the OSCs and leuco-RhoB correlates with binding energy, with N2200 exhibiting stronger binding than DPP-DTT. This enhanced interaction is consistent with improved spatial complementarity, contributing to the improved doping efficiency observed in N2200. Atomic force microscopy and x-ray diffraction analyses confirm better miscibility of leuco-RhoB with N2200, while electrical characterization demonstrates typical <i>n</i>-type doping effects. Leuco-RhoB-doped OSCs exhibit enhanced photoresponsive behavior with improved responsivity, external quantum efficiency, and detectivity, along with faster response times of 0.08&#xa0;s. These findings advance the rational design of <i>n</i>-type dopants by highlighting the importance of specific structural interactions with OSC beyond energy level alignment.</p> Graphical Abstract <p></p>

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Mechanistic elucidation of solution-processable n-type doping via rhodamine B for photoresponsive neuromorphic organic semiconductors

  • 期刊论文

  • 发表日期：

    2026年3月10日

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  • Yonghee Kim,
  • Min Hyuk Kim,
  • Seong Bin Woo,
  • Minseo Kim,
  • Jeong-Mo Choi,
  • Eun Kwang Lee

摘要

While organic semiconductors (OSCs) offer potential for next-generation electronics, n-type doping in solution-processed OSCs consistently lags behind p-type doping in efficiency, stability, and reproducibility. A fundamental limitation is the lack of a comprehensive understanding of specific molecular interactions between OSCs and dopants at the structural level. This study addresses this challenge by investigating leuco-Rhodamine B (leuco-RhoB) as an n-type dopant for two polymer OSCs of DPP-DTT and N2200. Combining experimental methods with density functional theory calculations, we elucidate the molecular interactions governing OSC-dopant binding preferences and their impact on electrical performance. Spatial overlap between the van der Waals volumes of the OSCs and leuco-RhoB correlates with binding energy, with N2200 exhibiting stronger binding than DPP-DTT. This enhanced interaction is consistent with improved spatial complementarity, contributing to the improved doping efficiency observed in N2200. Atomic force microscopy and x-ray diffraction analyses confirm better miscibility of leuco-RhoB with N2200, while electrical characterization demonstrates typical n-type doping effects. Leuco-RhoB-doped OSCs exhibit enhanced photoresponsive behavior with improved responsivity, external quantum efficiency, and detectivity, along with faster response times of 0.08 s. These findings advance the rational design of n-type dopants by highlighting the importance of specific structural interactions with OSC beyond energy level alignment.

Graphical Abstract