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具有激子/等离子体混合性质的全无机钙钛矿微腔中激发态和耦合机制的剧烈转变。

Drastic transitions of excited state and coupling regime in all-inorganic perovskite microcavities characterized by exciton/plasmon hybrid natures.

作者信息

Enomoto Shuki, Tagami Tomoya, Ueda Yusuke, Moriyama Yuta, Fujiwara Kentaro, Takahashi Shun, Yamashita Kenichi

机构信息

Faculty of Electrical Engineering and Electronics, Kyoto Institute of Technology, Matsugasaki, Sakyo-ku, Kyoto, 606-8585, Japan.

出版信息

Light Sci Appl. 2022 Jan 2;11(1):8. doi: 10.1038/s41377-021-00701-8.

Abstract

Lead-halide perovskites are highly promising for various optoelectronic applications, including laser devices. However, fundamental photophysics explaining the coherent-light emission from this material system is so intricate and often the subject of debate. Here, we systematically investigate photoluminescence properties of all-inorganic perovskite microcavity at room temperature and discuss the excited state and the light-matter coupling regime depending on excitation density. Angle-resolved photoluminescence clearly exhibits that the microcavity system shows a transition from weak coupling regime to strong coupling regime, revealing the increase in correlated electron-hole pairs. With pumping fluence above the threshold, the photoluminescence signal shows a lasing behavior with bosonic condensation characteristics, accompanied by long-range phase coherence. The excitation density required for the lasing behavior, however, is found to exceed the Mott density, excluding the exciton as the excited state. These results demonstrate that the polaritonic Bardeen-Cooper-Schrieffer state originates the strong coupling formation and the lasing behavior.

摘要

卤化铅钙钛矿在包括激光器件在内的各种光电器件应用中极具前景。然而,解释该材料系统相干光发射的基本光物理过程非常复杂,且常常是争论的焦点。在此,我们系统地研究了全无机钙钛矿微腔在室温下的光致发光特性,并根据激发密度讨论了激发态和光与物质的耦合机制。角分辨光致发光清楚地表明,微腔系统呈现出从弱耦合机制到强耦合机制的转变,这揭示了相关电子 - 空穴对数量的增加。当泵浦通量高于阈值时,光致发光信号呈现出具有玻色凝聚特性的激光行为,并伴有长程相位相干。然而,发现产生激光行为所需的激发密度超过了莫特密度,这排除了激子作为激发态的可能性。这些结果表明,极化子巴丁 - 库珀 - 施里弗尔态引发了强耦合的形成和激光行为。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5879/8720309/ad0274961d18/41377_2021_701_Fig1_HTML.jpg

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