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卤化铅钙钛矿量子点超晶格的超荧光

Superfluorescence from lead halide perovskite quantum dot superlattices.

作者信息

Rainò Gabriele, Becker Michael A, Bodnarchuk Maryna I, Mahrt Rainer F, Kovalenko Maksym V, Stöferle Thilo

机构信息

Department of Chemistry and Applied Bioscience, Institute of Inorganic Chemistry, ETH Zurich, Zurich, Switzerland.

Laboratory of Thin Films and Photovoltaics, Empa - Swiss Federal Laboratories for Materials Science and Technology, Dübendorf, Switzerland.

出版信息

Nature. 2018 Nov;563(7733):671-675. doi: 10.1038/s41586-018-0683-0. Epub 2018 Nov 7.

Abstract

An ensemble of emitters can behave very differently from its individual constituents when they interact coherently via a common light field. After excitation of such an ensemble, collective coupling can give rise to a many-body quantum phenomenon that results in short, intense bursts of light-so-called superfluorescence. Because this phenomenon requires a fine balance of interactions between the emitters and their decoupling from the environment, together with close identity of the individual emitters, superfluorescence has thus far been observed only in a limited number of systems, such as certain atomic and molecular gases and a few solid-state systems. The generation of superfluorescent light in colloidal nanocrystals (which are bright photonic sources practically suited for optoelectronics) has been precluded by inhomogeneous emission broadening, low oscillator strength, and fast exciton dephasing. Here we show that caesium lead halide (CsPbX, X = Cl, Br) perovskite nanocrystals that are self-organized into highly ordered three-dimensional superlattices exhibit key signatures of superfluorescence. These are dynamically red-shifted emission with more than 20-fold accelerated radiative decay, extension of the first-order coherence time by more than a factor of four, photon bunching, and delayed emission pulses with Burnham-Chiao ringing behaviour at high excitation density. These mesoscopically extended coherent states could be used to boost the performance of opto-electronic devices and enable entangled multi-photon quantum light sources.

摘要

当一组发光体通过共同的光场进行相干相互作用时,其行为可能与其单个组成部分有很大不同。在激发这样一组发光体后,集体耦合会引发一种多体量子现象,导致产生短暂而强烈的光脉冲——即所谓的超荧光。由于这种现象需要发光体之间的相互作用及其与环境的解耦达到精细平衡,同时单个发光体要非常相似,因此迄今为止,超荧光仅在有限数量的系统中被观测到,比如某些原子气体和分子气体以及少数固态系统。胶体纳米晶体(实际上是适用于光电子学的明亮光子源)中由于非均匀发射展宽、低振子强度和快速激子退相,一直无法产生超荧光。在此我们表明,自组装成高度有序三维超晶格的铯铅卤化物(CsPbX,X = Cl、Br)钙钛矿纳米晶体呈现出超荧光的关键特征。这些特征包括动态红移发射且辐射衰减加速20倍以上、一阶相干时间延长四倍以上、光子聚束以及在高激发密度下具有伯纳姆 - 乔(Burnham-Chiao)振荡行为的延迟发射脉冲。这些介观扩展的相干态可用于提高光电器件的性能,并实现纠缠多光子量子光源。

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