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首页> 外文期刊>Advanced energy materials >Why are Hot Holes Easier to Extract than Hot Electrons from Methylammonium Lead Iodide Perovskite?
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Why are Hot Holes Easier to Extract than Hot Electrons from Methylammonium Lead Iodide Perovskite?

机译：为什么热孔比从甲基铵碘化钙钛矿中的热电子更容易提取？

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摘要

Charge-carriers photoexcited above a semiconductor's bandgap rapidly thermalize to the band-edge. The cooling of these difficult to collect "hot" carriers caps the available photon energy that solar cells-including efficient perovskite solar cells-may utilize. Here, the dynamics and efficiency of hot carrier extraction from MAPbI(3) (MA = methylammonium) perovskite by spiro-OMeTAD (a hole-transporting layer) and TiO2 (an electron-transporting layer) are investigated and explained using both ultrafast electronic spectroscopy and theoretical modeling. Time-resolved spectroscopy reveals a quasi-equilibrium distribution of hot carriers forming upon excess-energy excitation of the perovskite-a distribution largely unaffected by the presence of TiO2. In contrast, the quasi-equilibrium distribution of hot carriers is virtually nonexistent when spiro-OMeTAD is present, which is indicative of efficient hot hole extraction at the interface of MAPbI(3). Density functional theory calculations predict that deep energy-levels of MAPbI(3) exhibit electronically delocalized character, with significant overlap with the localized valence band charge of the spiro-OMeTAD molecules lying on the surface of MAPbI(3). Consequently, hot holes are easily extracted from the deep energy-levels of MAPbI(3) by spiro-OMeTAD. These findings uncover the origins of efficient hot hole extraction in perovskites and offer a practical blueprint for optimizing solar cell interlayers to enable hot carrier utilization.
机译：在半导体带隙上方被光激发的电荷载流子迅速热化到带边。这些难以收集的“热”载流子的冷却限制了包括高效钙钛矿型太阳能电池在内的太阳能电池可利用的可用光子能量。在这里，研究和解释了使用Spiro-OMeTAD（空穴传输层）和TiO2（电子传输层）从MAPbI（3）（MA =甲基铵）钙钛矿中热载流子的萃取动力学和效率，并使用超快电子光谱学进行了解释。和理论建模。时间分辨光谱显示钙钛矿的过量能量激发后形成的热载流子的准平衡分布，这种分布在很大程度上不受TiO2的影响。相反，当存在螺旋OMeTAD时，热载流子的准平衡分布实际上不存在，这表明在MAPbI（3）的界面上有效地提取了热孔。密度泛函理论计算预测，MAPbI（3）的深能级表现出电子离域特征，与位于MAPbI（3）表面的螺-OMeTAD分子的局部价带电荷显着重叠。因此，通过螺-OMeTAD可以轻松地从MAPbI（3）的深能级中提取热孔。这些发现揭示了钙钛矿中有效热孔萃取的起源，并为优化太阳能电池夹层以实现热载流子利用提供了实用的蓝图。

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  • 来源
    《Advanced energy materials》 |2019年第22期|1900084.1-1900084.8|共8页
  • 作者

    Dursun Ibrahim; Maity Partha; Yin Jun; Turedi Bekir; Zhumekenov Ayan A.; Lee Kwang Jae; Mohammed Omar F.; Bakr Osman M.;

  • 作者单位

    KAUST, Div Phys Sci & Engn PSE, Thuwal 23955, Saudi Arabia|KAUST, Div Phys Sci & Engn PSE, KAUST Catalysis Ctr KCC, Thuwal 23955, Saudi Arabia;

    KAUST, Div Phys Sci & Engn PSE, Thuwal 23955, Saudi Arabia;

    KAUST, Div Phys Sci & Engn PSE, Thuwal 23955, Saudi Arabia;

    KAUST, Div Phys Sci & Engn PSE, Thuwal 23955, Saudi Arabia|KAUST, Div Phys Sci & Engn PSE, KAUST Catalysis Ctr KCC, Thuwal 23955, Saudi Arabia;

    KAUST, Div Phys Sci & Engn PSE, Thuwal 23955, Saudi Arabia|KAUST, Div Phys Sci & Engn PSE, KAUST Catalysis Ctr KCC, Thuwal 23955, Saudi Arabia;

    KAUST, Div Phys Sci & Engn PSE, Thuwal 23955, Saudi Arabia|KAUST, Div Phys Sci & Engn PSE, KAUST Catalysis Ctr KCC, Thuwal 23955, Saudi Arabia;

    KAUST, Div Phys Sci & Engn PSE, Thuwal 23955, Saudi Arabia;

    KAUST, Div Phys Sci & Engn PSE, Thuwal 23955, Saudi Arabia|KAUST, Div Phys Sci & Engn PSE, KAUST Catalysis Ctr KCC, Thuwal 23955, Saudi Arabia;

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  • 关键词

    carrier extraction; carrier temperature; density functional theory; halide perovskites; hot carriers;

    机译：载体提取;载体温度;密度函数理论;卤化物佩洛斯库茨;热载体;

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