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<p>Mixed-halide wide-bandgap (WBG) perovskites needed in tandem photovoltaics suffer from phase segregation, even at the time of initial film formation – the result of asymmetric nucleation of I-rich and Br-rich phases<sup>1-3</sup>. Known homogenization strategies tune Pb<sup>2+</sup> coordination strength<sup>4-6</sup>; however, Pb<sup>2+</sup>-based modulation applies across all Pb<sup>2+</sup> centers and does not preferentially address the problem that PbBr<sub>x</sub> nucleates faster than does PbI<sub>x</sub>. Here we introduce a selective coordination principle: we tune local Lewis-base hardness at the donor atom through a molecular dipole, an approach that constrains the polarizability of the O-donor’s outermost electrons. The harder O-donor preferentially coordinates the harder Pb<sup>2+</sup> of PbBr<sub>x</sub>, selectively retarding Br-rich nucleation and synchronizing it with PbI<sub>x</sub>. This leads to compositionally homogeneous WBG films, enabling solar cells with bandgaps of 1.62 eV, 1.68 eV, and 1.88 eV, each achieving enhanced PCE and extended stability (1500 h, ≥<i>T</i><sub>90</sub>, 1 sun and 65 °C). Perovskite/organic tandem cells fabricated with these WBG films and an infrared-active organic cell deliver certified 27.0% (steady-state 26.4%) efficiency, with <i>T</i><sub>91</sub> (ISOS-L2 at 65 °C) of 1000 h.</p>

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Phase-homogeneous mixed halide perovskites for stable tandem photovoltaics

  • 期刊论文

  • 发表日期：

    2026年7月27日

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  • Pengju Shi,
  • Jiale Zhuang,
  • Dayong Zhang,
  • Chu Li,
  • Stefan Zeiske,
  • Jin Hou,
  • Isaiah W. Gilley,
  • Ilhan Yavuz,
  • Ubaid Kazianga,
  • Congqi Li,
  • Yu Zhang,
  • Kefu Huang,
  • Teerapat Itsoponpan,
  • Xin Jiang,
  • Chiung-Han Chen,
  • Chuying Huang,
  • Yi Yang,
  • Xianfu Zhang,
  • Pronoy Nandi,
  • Samantha A. Reitz,
  • Antonio Facchetti,
  • Keith P. White,
  • Keenan Wyatt,
  • Michael F. Toney,
  • Mercouri G. Kanatzidis,
  • Tobin J. Marks,
  • Cheng Liu,
  • Bin Chen,
  • Edward H. Sargent

摘要

Mixed-halide wide-bandgap (WBG) perovskites needed in tandem photovoltaics suffer from phase segregation, even at the time of initial film formation – the result of asymmetric nucleation of I-rich and Br-rich phases1-3. Known homogenization strategies tune Pb2+ coordination strength4-6; however, Pb2+-based modulation applies across all Pb2+ centers and does not preferentially address the problem that PbBrx nucleates faster than does PbIx. Here we introduce a selective coordination principle: we tune local Lewis-base hardness at the donor atom through a molecular dipole, an approach that constrains the polarizability of the O-donor’s outermost electrons. The harder O-donor preferentially coordinates the harder Pb2+ of PbBrx, selectively retarding Br-rich nucleation and synchronizing it with PbIx. This leads to compositionally homogeneous WBG films, enabling solar cells with bandgaps of 1.62 eV, 1.68 eV, and 1.88 eV, each achieving enhanced PCE and extended stability (1500 h, ≥T90, 1 sun and 65 °C). Perovskite/organic tandem cells fabricated with these WBG films and an infrared-active organic cell deliver certified 27.0% (steady-state 26.4%) efficiency, with T91 (ISOS-L2 at 65 °C) of 1000 h.