arXiv 2603.182632026-03-31cond-mat.mtrl-sci

锌多磷酸盐中稳定的长光激发载流子寿命

Long photoexcited carrier lifetime in a stable and earth-abundant zinc polyphosphide

Thayer School of Engineering, Dartmouth College（达特茅斯学院泰勒工程学院）；Department of Materials Science and NanoEngineering, Rice University（莱斯大学材料科学与纳米工程系）；Rice Advanced Materials Institute, Rice University（莱斯大学莱斯先进材料研究所）；Department of Chemistry, Iowa State University（爱荷华州立大学化学系）；National Laboratory of the Rockies, U.S. Department of Energy（美国能源部落基山国家实验室）；Department of Physics and Astronomy, Dartmouth College（达特茅斯学院物理与天文系）；Aiiso Yufeng Li Family Department of Chemical and Nano Engineering, University of California San Diego（加州大学圣地亚哥分校艾索余峰李家族化学与纳米工程系）；Ames National Laboratory, U.S. Department of Energy（美国能源部艾姆斯国家实验室）；Renewable and Sustainable Energy Institute, University of Colorado Boulder（科罗拉多大学博尔德分校可再生与可持续能源研究所）

Zhenkun Yuan, Genevieve Amobi, Shaham Quadir, Smitakshi Goswami, Guillermo L. Esparza, Gideon Kassa, Gayatri Viswanathan, Joseph T. Race, Muhammad R. Hasan, Jac… 展开作者

Zhenkun Yuan, Genevieve Amobi, Shaham Quadir, Smitakshi Goswami, Guillermo L. Esparza, Gideon Kassa, Gayatri Viswanathan, Joseph T. Race, Muhammad R. Hasan, Jack R. Palmer, Sita Dugu, Yagmur Coban, Andriy Zakutayev, Obadiah G. Reid, David P. Fenning, Kirill Kovnir, Sage R. Bauers, Jifeng Liu, Geoffroy Hautier

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AI总结：

研究发现锌多磷酸盐具有极长的光激发载流子寿命，填补了直接带隙无机半导体与卤化物钙钛矿之间的载流子寿命差距，其独特的多磷酸键结构抑制了深内在缺陷的形成，展现出优异的环境稳定性。

摘要：

卤化物钙钛矿通过在相对不严格的加工环境下实现长载流子寿命，而传统无机半导体通常需要精心制备和后处理才能获得较长的载流子寿命。本文报告了单斜锌多磷酸盐（ZnP2）中异常长的光激发载流子寿命，有效弥合了直接带隙无机半导体与卤化物钙钛矿之间的载流子寿命差距。通过计算筛选，ZnP2被识别为具有非传统多磷酸键结构的长载流子寿命半导体，其结合共价结合的磷链和极性共价的Zn-P四面体。实验上，由低纯度前驱体合成的ZnP2晶体表现出1.49 eV的明亮带间发光和高达1 μs的载流子寿命。进一步分析显示，ZnP2的多磷酸键抑制了深内在缺陷的形成，使其具有抗缺陷性。结合其显著的环境稳定性，ZnP2成为太阳能吸收体和发光体的有前途的材料。本工作表明，未被充分探索的无机材料空间中具有不寻常化学键的材料在发现新型光电材料方面具有巨大潜力。

英文摘要：

Halide perovskites have revolutionized optoelectronics by demonstrating that long carrier lifetime can be achieved in materials processed in relatively uncontrolled environments, whereas conventional inorganic semiconductors typically suffer from short carrier lifetime unless very carefully prepared and postprocessed. Here, we report the discovery of exceptionally long photoexcited carrier lifetime in monoclinic ZnP2, effectively bridging the carrier lifetime gap between direct-gap inorganic semiconductors and halide perovskites. Through computational screening, ZnP2 is identified as a long carrier lifetime semiconductor characterized by an unconventional polyphosphide bonding, combining covalently bonded phosphorus chains and polar-covalent Zn-P tetrahedra. Experimentally, ZnP2 crystals synthesized from low-purity precursors exhibit bright band-to-band photoluminescence at 1.49 eV and carrier lifetimes of up to 1 $μ$s. Further analysis reveals that the polyphosphide bonding of ZnP2 suppresses the formation of deep intrinsic defects, making it defect resistant. Combined with its remarkable environmental stability, ZnP2 presents a highly promising material for solar absorbers and light emitters. Our work illustrates that underexplored inorganic materials spaces with unusual chemical bonding hold great promise for discovering novel optoelectronic materials.

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