Bright triplet excitons in caesium lead halide perovskites

激子 半导体 比克西顿 卤化物 纳米晶 钙钛矿(结构) 吸收(声学) 材料科学 光电子学 原子物理学 化学 凝聚态物理 物理 纳米技术 无机化学 结晶学 复合材料
作者
Michael A. Becker,Roman Vaxenburg,Georgian Nedelcu,Peter C. Sercel,Andrew Shabaev,Michael J. Mehl,John G. Michopoulos,Samuel G. Lambrakos,Noam Bernstein,John L. Lyons,Thilo Stöferle,Rainer F. Mahrt,Maksym V. Kovalenko,David J. Norris,Gabriele Rainò,Alexander L. Efros
出处
期刊:Nature [Nature Portfolio]
卷期号:553 (7687): 189-193 被引量:888
标识
DOI:10.1038/nature25147
摘要

Nanostructured semiconductors emit light from electronic states known as excitons[1]. According to Hund's rules[2], the lowest energy exciton in organic materials should be a poorly emitting triplet state. Analogously, the lowest exciton level in all known inorganic semiconductors is believed to be optically inactive. These 'dark' excitons (into which the system can relax) hinder light-emitting devices based on semiconductor nanostructures. While strategies to diminish their influence have been developed[3-5], no materials have been identified in which the lowest exciton is bright. Here we show that the lowest exciton in quasi-cubic lead halide perovskites is optically active. We first use the effective-mass model and group theory to explore this possibility, which can occur when the strong spin-orbit coupling in the perovskite conduction band is combined with the Rashba effect [6-10]. We then apply our model to CsPbX3 (X=Cl,Br,I) nanocrystals[11], for which we measure size- and composition-dependent fluorescence at the single-nanocrystal level. The bright character of the lowest exciton immediately explains the anomalous photon-emission rates of these materials, which emit 20 and 1,000 times faster[12] than any other semiconductor nanocrystal at room[13-16] and cryogenic[17] temperatures, respectively. The bright exciton is further confirmed by detailed analysis of the fine structure in low-temperature fluorescence spectra. For semiconductor nanocrystals[18], which are already used in lighting[19,20], lasers[21,22], and displays[23], these optically active excitons can lead to materials with brighter emission and enhanced absorption. More generally, our results provide criteria for identifying other semiconductors exhibiting bright excitons with potentially broad implications for optoelectronic devices.
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