Bimolecular recombination in methylammonium lead triiodide perovskite is an inverse absorption process.
Bimolecular recombination in methylammonium lead triiodide perovskite is an inverse absorption process.
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三二二二二二二二二二何二二二二二二二二二酯铅的双分子重组是一个反吸收过程。
DOI：
10.1038/s41467-017-02670-2
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发表时间：
2018-01-18
影响因子：
16.6
通讯作者：
Herz LM
中科院分区：
文献类型：
--
作者：
Davies CL;Filip MR;Patel JB;Crothers TW;Verdi C;Wright AD;Milot RL;Giustino F;Johnston MB;Herz LM
基于金属卤化物钙钛矿的光伏器件在效率上迅速提高。一旦达到肖克利-奎塞尔极限，电荷载流子的提取将只受到电子与空穴的辐射双分子复合的限制。然而，这一基本过程及其与材料化学计量的联系仍然知之甚少。在这里，我们表明，在甲基铵三碘化铅钙钛矿双分子电荷载流子复合可以完全解释为吸收的逆过程。通过正确考虑激子和电子-空穴连续态对吸收的贡献，我们能够利用货车Roosbroeck-Shockley关系从吸收光谱确定双分子复合速率常数。我们发现，锐化的光子，电子和空穴分布函数显着增强双分子电荷复合的温度降低，反映在瞬态光谱的趋势。我们的研究结果提供了对这种混合钙钛矿中带间复合过程的重要理解，该过程包括热化电子和空穴之间的直接，完全辐射跃迁。辐射双分子过程将主导混合钙钛矿太阳能电池在肖克利-奎塞尔极限附近工作的电荷载流子复合。在这里，作者表明，这样的过程是吸收的逆，并随着分布函数向较低温度的尖锐化而增加。
Photovoltaic devices based on metal halide perovskites are rapidly improving in efficiency. Once the Shockley–Queisser limit is reached, charge-carrier extraction will be limited only by radiative bimolecular recombination of electrons with holes. Yet, this fundamental process, and its link with material stoichiometry, is still poorly understood. Here we show that bimolecular charge-carrier recombination in methylammonium lead triiodide perovskite can be fully explained as the inverse process of absorption. By correctly accounting for contributions to the absorption from excitons and electron-hole continuum states, we are able to utilise the van Roosbroeck–Shockley relation to determine bimolecular recombination rate constants from absorption spectra. We show that the sharpening of photon, electron and hole distribution functions significantly enhances bimolecular charge recombination as the temperature is lowered, mirroring trends in transient spectroscopy. Our findings provide vital understanding of band-to-band recombination processes in this hybrid perovskite, which comprise direct, fully radiative transitions between thermalized electrons and holes. Radiative bimolecular processes will dominate charge-carrier recombination in hybrid perovskite solar cells operating near the Shockley-Queisser limit. Here, the authors show that such processes are the inverse of absorption and increase as distribution functions sharpen towards lower temperatures.
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影响因子：
6.7
作者：
Green, Martin A.;Emery, Keith;Ho-Baillie, Anita W. Y.
通讯作者：
Ho-Baillie, Anita W. Y.
影响因子：
22
作者：
Kirchartz, Thomas;Staub, Florian;Rau, Uwe
通讯作者：
Rau, Uwe
影响因子：
35
作者：
Manser, Joseph S.;Kamat, Prashant V.
通讯作者：
Kamat, Prashant V.
影响因子：
3.7
作者：
Filippetti, Alessio;Delugas, Pietro;Mattoni, Alessandro
通讯作者：
Mattoni, Alessandro
影响因子：
6.1
作者：
Kandada, Ajay Ram Srimath;Petrozza, Annamaria
通讯作者：
Petrozza, Annamaria