Thermal Decoherence of Superradiance in Lead Halide Perovskite Nanocrystal Superlattices
Thermal Decoherence of Superradiance in Lead Halide Perovskite Nanocrystal Superlattices
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DOI：
10.1021/acs.nanolett.0c02784
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发表时间：
2020-10-14
期刊：
影响因子：
10.8
通讯作者：
Luca Celardo, G.
中科院分区：
文献类型：
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作者：
Mattiotti, Francesco;Kuno, Masaru;Luca Celardo, G.
Raino等人最近的实验。(自然2018,563,671-675)记录了CsPbBr3纳米晶体超晶格的合作发射，显示出低温超辐射的特征。特别是，光学响应是相干的，辐射衰减率比单个纳米晶体的辐射衰减率增加了3倍。然而，这一增加比由10(6)-10(8)个相互作用的纳米晶体组成的大型组件的超辐射理论预期要小6个数量级。在这里，我们建立了这类系统的超辐射理论模型，并证明了热退相干是导致纳米晶超晶格辐射衰减率急剧降低的主要原因。我们的理论方法解释了实验结果(《自然》2018,563,671-675)，为小型纳米超晶格的设计提供了洞察，并显示出超辐射响应的4个数量级的增强。这些定量预测为在更高温度下观测超辐射铺平了道路。
Recent experiments by Raino` et al. (Nature 2018, 563, 671-675) have documented cooperative emission from CsPbBr3 nanocrystal superlattices, exhibiting the hallmarks of low-temperature superradiance. In particular, the optical response is coherent and the radiative decay rate is increased by a factor of 3, relative to that of individual nanocrystals. However, the increase is 6 orders of magnitude smaller than what is theoretically expected from the superradiance of large assemblies, consisting of 10(6)-10(8) interacting nanocrystals. Here, we develop a theoretical model of superradiance for such systems and show that thermal decoherence is largely responsible for the drastic reduction of the radiative decay rate in nanocrystal superlattices. Our theoretical approach explains the experimental results (Nature 2018, 563, 671-675), provides insight into the design of small nanocrystal superlattices, and shows a 4 orders of magnitude enhancement in superradiant response. These quantitative predictions pave the path toward observing superradiance at higher temperatures.