Cho Kenichi, Tahara Hirokazu, Yamada Takumi, Suzuura Hidekatsu, Tadano Terumasa, Sato Ryota, Saruyama Masaki, Hirori Hideki, Teranishi Toshiharu, Kanemitsu Yoshihiko
Institute for Chemical Research, Kyoto University, Uji, Kyoto 611-0011, Japan.
The Hakubi Center for Advanced Research, Kyoto University, Kyoto 606-8501, Japan.
Nano Lett. 2022 Sep 28;22(18):7674-7681. doi: 10.1021/acs.nanolett.2c02970. Epub 2022 Sep 19.
Lead halide perovskite nanocrystals (NCs) have outstanding photoluminescence (PL) properties and excellent potential for light-emitting diodes and single-photon sources. Here, we report the multiple-peak structures originating from excitons, trions, and biexcitons in low-temperature PL spectra of single CsPbBr NCs. We found fine-structure splitting in the PL peaks of bright excitons and biexcitons and also in the longitudinal-optical (LO)-phonon replicas of excitons. LO-phonon replicas of trions are clearly observed under strong photoexcitation, which do not show fine-structure splitting. From size-dependent analyses of these replicas, we clarified that both exciton-phonon and trion-phonon couplings become larger for smaller NCs and the coupling strengths of trions are larger than those of excitons in large NCs. These behaviors can be explained by the spatial distributions of the electron and hole wave functions in the NCs. Our findings provide essential information on electron-phonon couplings in perovskites and for the design of high-purity single-photon sources.
卤化铅钙钛矿纳米晶体(NCs)具有出色的光致发光(PL)特性,在发光二极管和单光子源方面具有优异的潜力。在此,我们报告了单个CsPbBr NCs低温PL光谱中源自激子、三重态激子和双激子的多峰结构。我们发现明亮激子和双激子的PL峰以及激子的纵向光学(LO)声子复制品中存在精细结构分裂。在强光激发下可以清楚地观察到三重态激子的LO声子复制品,其没有显示出精细结构分裂。通过对这些复制品的尺寸依赖性分析,我们阐明了对于较小的NCs,激子 - 声子和三重态激子 - 声子耦合都变得更大,并且在大尺寸NCs中三重态激子的耦合强度大于激子的耦合强度。这些行为可以通过NCs中电子和空穴波函数的空间分布来解释。我们的发现为钙钛矿中的电子 - 声子耦合以及高纯度单光子源的设计提供了重要信息。