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<p>Double perovskite films offer significant potential for multiferroic and ferroelectric photovoltaics due to their structural tunability. This study employs an aliovalent substitution strategy, partially replacing Bi with Pb in Bi<sub>2</sub>FeMnO<sub>6</sub> (BFMO), to disrupt charge balance and local polarization while maintaining the host lattice. Pb incorporation simultaneously modulates the chemical states of all constituent elements, inducing pronounced lattice distortion and positive chemical strain. Unpoled Pb-BFMO films exhibit exceptional photovoltaic performance under 80 mW cm<sup>−2</sup> illumination, achieving a short-circuit current density (|<i>J</i><sub>SC</sub>|) of 192&#xa0;μA&#xa0;cm<sup>−2</sup> and an open-circuit voltage (|<i>V</i><sub>OC</sub>|) of 0.525&#xa0;V. This represents a 109-fold increase in intrinsic <i>J</i><sub>SC</sub> and a fourfold enhancement in V<sub>OC</sub> compared to pure BFMO. The |<i>J</i><sub>SC</sub>| demonstrates electric field tunability via polarization switching, reaching 320&#xa0;μA&#xa0;cm<sup>−2</sup> under negative polarization, the highest reported <i>J</i><sub>SC</sub> for sub-100&#xa0;nm single-layer ferroelectric films under white light. High-resolution high-angle annular dark-field scanning transmission electron microscopy, synchrotron-based reciprocal space mapping and X-ray absorption spectroscopy analyses collectively confirm the coupling of crystal distortion, chemical strain, and valence state alterations. The synergy between chemical strain and ionic valence states effectively engineers the bandgap and enhances photovoltaic response, which unlocks new application pathways for perovskite materials in optical memory devices and sustainable energy systems.</p>

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Chemo-Strain Valence Engineering for Boosting Photovoltaic Response in Double Perovskite Epitaxial Films

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月4日

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  • Yonghui Wu,
  • Jie Tu,
  • Jing Xia,
  • Xudong Liu,
  • Longyuan Shi,
  • Hangren Li,
  • Menglin Li,
  • Peng Chen,
  • Qianqian Yang,
  • Siyuan Du,
  • Pengfei Song,
  • Haiying Li,
  • Qian Zhan,
  • Xiaolong Li,
  • Jianjun Tian,
  • Linxing Zhang

摘要

Double perovskite films offer significant potential for multiferroic and ferroelectric photovoltaics due to their structural tunability. This study employs an aliovalent substitution strategy, partially replacing Bi with Pb in Bi2FeMnO6 (BFMO), to disrupt charge balance and local polarization while maintaining the host lattice. Pb incorporation simultaneously modulates the chemical states of all constituent elements, inducing pronounced lattice distortion and positive chemical strain. Unpoled Pb-BFMO films exhibit exceptional photovoltaic performance under 80 mW cm−2 illumination, achieving a short-circuit current density (|JSC|) of 192 μA cm−2 and an open-circuit voltage (|VOC|) of 0.525 V. This represents a 109-fold increase in intrinsic JSC and a fourfold enhancement in VOC compared to pure BFMO. The |JSC| demonstrates electric field tunability via polarization switching, reaching 320 μA cm−2 under negative polarization, the highest reported JSC for sub-100 nm single-layer ferroelectric films under white light. High-resolution high-angle annular dark-field scanning transmission electron microscopy, synchrotron-based reciprocal space mapping and X-ray absorption spectroscopy analyses collectively confirm the coupling of crystal distortion, chemical strain, and valence state alterations. The synergy between chemical strain and ionic valence states effectively engineers the bandgap and enhances photovoltaic response, which unlocks new application pathways for perovskite materials in optical memory devices and sustainable energy systems.