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Charge-Carrier Recombination in Halide Perovskites.
Chemical Reviews ( IF 51.4 ) Pub Date : 2019-09-09 , DOI: 10.1021/acs.chemrev.9b00169
Dane W deQuilettes 1, 2 , Kyle Frohna 3 , David Emin 4 , Thomas Kirchartz 5, 6 , Vladimir Bulovic 1 , David S Ginger 2 , Samuel D Stranks 3
Chemical Reviews ( IF 51.4 ) Pub Date : 2019-09-09 , DOI: 10.1021/acs.chemrev.9b00169
Dane W deQuilettes 1, 2 , Kyle Frohna 3 , David Emin 4 , Thomas Kirchartz 5, 6 , Vladimir Bulovic 1 , David S Ginger 2 , Samuel D Stranks 3
Affiliation
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The success of halide perovskites in a host of optoelectronic applications is often attributed to their long photoexcited carrier lifetimes, which has led to charge-carrier recombination processes being described as unique compared to other semiconductors. Here, we integrate recent literature findings to provide a critical assessment of the factors we believe are most likely controlling recombination in the most widely studied halide perovskite systems. We focus on four mechanisms that have been proposed to affect measured charge carrier recombination lifetimes, namely: (1) recombination via trap states, (2) polaron formation, (3) the indirect nature of the bandgap (e.g., Rashba effect), and (4) photon recycling. We scrutinize the evidence for each case and the implications of each process on carrier recombination dynamics. Although they have attracted considerable speculation, we conclude that multiple trapping or hopping in shallow trap states, and the possible indirect nature of the bandgap (e.g., Rashba effect), seem to be less likely given the combined evidence, at least in high-quality samples most relevant to solar cells and light-emitting diodes. On the other hand, photon recycling appears to play a clear role in increasing apparent lifetime for samples with high photoluminescence quantum yields. We conclude that polaron dynamics are intriguing and deserving of further study. We highlight potential interdependencies of these processes and suggest future experiments to better decouple their relative contributions. A more complete understanding of the recombination processes could allow us to rationally tailor the properties of these fascinating semiconductors and will aid the discovery of other materials exhibiting similarly exceptional optoelectronic properties.
中文翻译：
卤化物钙钛矿中的电荷-载流子复合。
卤化物钙钛矿在许多光电应用中的成功通常归因于其长的光激发载流子寿命，这导致电荷载流子复合过程被描述为与其他半导体相比具有独特性。在这里，我们综合了最近的文献发现，以对我们认为最有可能在最广泛研究的卤化物钙钛矿体系中控制重组的因素进行关键评估。我们关注于已提出的影响测得的电荷载流子复合寿命的四种机制，即：（1）通过陷阱态进行的复合，（2）极化子形成，（3）带隙的间接性质（例如，拉什巴效应）和（4）光子回收。我们仔细研究每种情况的证据以及每个过程对载体重组动力学的影响。尽管它们引起了相当大的猜测，但我们得出的结论是，鉴于综合的证据，至少在高质量条件下，在浅陷阱状态中的多次陷波或跳跃以及带隙的可能间接性质（例如，拉什巴效应）似乎不太可能。与太阳能电池和发光二极管最相关的样本。另一方面，对于具有高光致发光量子产率的样品，光子回收似乎在增加其表观寿命方面起着明显的作用。我们得出的结论是，极化子动力学令人着迷，值得进一步研究。我们重点介绍了这些过程之间的潜在相互依存关系，并建议未来进行实验以更好地分离它们的相对贡献。
更新日期：2019-09-09
中文翻译：
卤化物钙钛矿中的电荷-载流子复合。
卤化物钙钛矿在许多光电应用中的成功通常归因于其长的光激发载流子寿命，这导致电荷载流子复合过程被描述为与其他半导体相比具有独特性。在这里，我们综合了最近的文献发现，以对我们认为最有可能在最广泛研究的卤化物钙钛矿体系中控制重组的因素进行关键评估。我们关注于已提出的影响测得的电荷载流子复合寿命的四种机制，即：（1）通过陷阱态进行的复合，（2）极化子形成，（3）带隙的间接性质（例如，拉什巴效应）和（4）光子回收。我们仔细研究每种情况的证据以及每个过程对载体重组动力学的影响。尽管它们引起了相当大的猜测，但我们得出的结论是，鉴于综合的证据，至少在高质量条件下，在浅陷阱状态中的多次陷波或跳跃以及带隙的可能间接性质（例如，拉什巴效应）似乎不太可能。与太阳能电池和发光二极管最相关的样本。另一方面，对于具有高光致发光量子产率的样品，光子回收似乎在增加其表观寿命方面起着明显的作用。我们得出的结论是，极化子动力学令人着迷，值得进一步研究。我们重点介绍了这些过程之间的潜在相互依存关系，并建议未来进行实验以更好地分离它们的相对贡献。
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