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Impact of Crystal Surface on Photoexcited States in Organic-Inorganic Perovskites

机译：晶体表面对有机无机钙钛矿中光激发态的影响

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Despite their outstanding photovoltaic performance, organic-inorganic perovskite solar cells still face severe stability issues and limitations in their device dimension. Further development of perovskite solar cells therefore requires a deeper understanding of loss mechanisms, in particular, concerning the origin and impact of trap states. Here, different surface properties of submicrometer sized CH3NH3PbI3 particles are studied as a model system by photoluminescence spectroscopy to investigate the impact of the perovskite crystal surface on photoexcited states. Comparison of single crystals with either isolating or electron-rich surface passivation indicates the presence of positively charged surface trap states that can be passivated in case of the latter. These surface trap states cause enhanced nonradiative recombination at room temperature, which is a loss mechanism for solar cell performance. In the orthorhombic phase, the origin of multiple emission peaks is identified as the recombination of free and bound excitons, whose population ratio critically depends on trap state properties. The dynamics of exciton trapping at 50 K are observed on a time-scale of tens of picoseconds by a simultaneous population decrease and increase of free and bound excitons, respectively. These results emphasize the potential of surface passivation to further improve the performance of perovskite solar cells.
机译：尽管其出色的光伏性能，有机-无机钙钛矿太阳能电池仍面临严重的稳定性问题和器件尺寸方面的限制。因此，钙钛矿太阳能电池的进一步发展需要对损失机理有更深入的了解，尤其是关于陷阱态的起源和影响。在这里，通过光致发光光谱法研究了亚微米尺寸的CH3NH3PbI3颗粒的不同表面性质，作为模型系统，以研究钙钛矿晶体表面对光激发态的影响。具有隔离或富电子表面钝化的单晶的比较表明存在带正电的表面陷阱态，在后者的情况下可以被钝化。这些表面陷阱状态导致室温下增强的非辐射复合，这是太阳能电池性能的损失机制。在正交相阶段，多个发射峰的起源被确定为自由和束缚激子的复合，激子的种群比例主要取决于陷阱态的性质。在数十皮秒的时间尺度上观察到了激子在50 K处的俘获动力学，这是由于游离激子和结合激子分别同时减少和增加。这些结果强调了表面钝化的潜力，以进一步改善钙钛矿太阳能电池的性能。

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  • 来源
    《Advanced Functional Materials》 |2017年第6期|1604995.1-1604995.9|共9页
  • 作者

    Birkhold Susanne T.; Zimmermann Eugen; Kollek Tom; Wurmbrand Daniel; Polarz Sebastian; Schmidt-Mende Lukas;

  • 作者单位

    Univ Konstanz, Dept Phys, Univ Str 10, D-78457 Constance, Germany;

    Univ Konstanz, Dept Phys, Univ Str 10, D-78457 Constance, Germany;

    Univ Konstanz, Dept Chem, Univ Str 10, D-78457 Constance, Germany;

    Univ Konstanz, Dept Chem, Univ Str 10, D-78457 Constance, Germany;

    Univ Konstanz, Dept Chem, Univ Str 10, D-78457 Constance, Germany;

    Univ Konstanz, Dept Phys, Univ Str 10, D-78457 Constance, Germany;

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