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<p>Organic photovoltaics (OPVs) that operate efficiently under both outdoor and indoor conditions remain challenging because the governing requirements for spectral absorption, energy-level alignment, and recombination suppression differ fundamentally among these conditions. Here, we report a pyrimido[5,4-<i>d</i>]pyrimidine (PyPy)-based π-conjugated polymer, <b>P(PyPy-BDT)</b>, as a versatile wide-bandgap donor enabling dual-mode OPVs. The incorporation of the strongly electron-deficient PyPy unit deepens the HOMO level, resulting in high open-circuit voltages of up to 0.93 and 1.21 V when combined with the nonfullerene acceptors <b>IT-4F</b> and <b>IO-4F</b>, respectively. Under standard 1-sun illumination, <b>P(PyPy-BDT):IT-4F</b>-based devices achieved a higher power conversion efficiency (PCE) of 9.3% compared with the corresponding <b>IO-4F</b>-based devices. In contrast, under indoor dim-light conditions, the performance trend was reversed: <b>P(PyPy-BDT):IO-4F</b>-based devices delivered a high PCE of 20.0%, outperforming <b>IT-4F</b>-based devices under a white LED at 1000 lx. This inversion originates from the combined effects of spectral matching, energetic alignment, and recombination dynamics, which govern device operation differently under distinct illumination conditions. These results highlight the illumination-dependent nature of OPV performance and provide a general design guideline for dual-mode OPVs, offering a viable pathway toward high-performance indoor energy harvesting.</p>

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Efficient indoor and outdoor organic photovoltaics enabled by a pyrimido[5,4-d]pyrimidine-based π-conjugated polymer

  • 期刊论文

  • 发表日期：

    2026年5月22日

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  • Jiahui Duan,
  • Asumi Sueyasu,
  • Takuma Yasuda

摘要

Organic photovoltaics (OPVs) that operate efficiently under both outdoor and indoor conditions remain challenging because the governing requirements for spectral absorption, energy-level alignment, and recombination suppression differ fundamentally among these conditions. Here, we report a pyrimido[5,4-d]pyrimidine (PyPy)-based π-conjugated polymer, P(PyPy-BDT), as a versatile wide-bandgap donor enabling dual-mode OPVs. The incorporation of the strongly electron-deficient PyPy unit deepens the HOMO level, resulting in high open-circuit voltages of up to 0.93 and 1.21 V when combined with the nonfullerene acceptors IT-4F and IO-4F, respectively. Under standard 1-sun illumination, P(PyPy-BDT):IT-4F-based devices achieved a higher power conversion efficiency (PCE) of 9.3% compared with the corresponding IO-4F-based devices. In contrast, under indoor dim-light conditions, the performance trend was reversed: P(PyPy-BDT):IO-4F-based devices delivered a high PCE of 20.0%, outperforming IT-4F-based devices under a white LED at 1000 lx. This inversion originates from the combined effects of spectral matching, energetic alignment, and recombination dynamics, which govern device operation differently under distinct illumination conditions. These results highlight the illumination-dependent nature of OPV performance and provide a general design guideline for dual-mode OPVs, offering a viable pathway toward high-performance indoor energy harvesting.