Chuang Yung-Tang, Lin Tzu-Yu, Tan Guang-Hsun, Jan Pei-En, Lin Hao-Cheng, Chen Hung-Ming, Hsiao Kai-Yuan, Chen Bo-Han, Lu Chih-Hsuan, Lee Chi-Hsuan, Pao Chun-Wei, Yang Shang-Da, Lu Ming-Yen, Lin Hao-Wu
Department of Materials Science and Engineering, National Tsing Hua University, Hsinchu, 30013, Taiwan.
Institute of Photonics Technologies, National Tsing Hua University, Hsinchu, 30013, Taiwan.
Small. 2024 May;20(18):e2308676. doi: 10.1002/smll.202308676. Epub 2023 Dec 10.
Highly emissive semiconductor nanocrystals, or so-called quantum dots (QDs) possess a variety of applications from displays and biology labeling, to quantum communication and modern security. Though ensembles of QDs have already shown very high photoluminescent quantum yields (PLQYs) and have been widely utilized in current optoelectronic products, QDs that exhibit high absorption cross-section, high emission intensity, and, most important, nonblinking behavior at single-dot level have long been desired and not yet realized at room temperature. In this work, infrared-emissive MAPbI-based halide perovskite QDs is demonstrated. These QDs not only show a ≈100% PLQY at the ensemble level but also, surprisingly, at the single-dot level, display an extra-large absorption cross-section up to 1.80 × 10 cm and non-blinking single photon emission with a high single photon purity of 95.3%, a unique property that is extremely rare among all types of quantum emitters operated at room temperature. An in-depth analysis indicates that neither trion formation nor band-edge carrier trapping is observed in MAPbI QDs, resulting in the suppression of intensity blinking and lifetime blinking. Fluence-dependent transient absorption measurements reveal that the coexistence of non-blinking behavior and high single photon purity in these perovskite QDs results from a significant repulsive exciton-exciton interaction, which suppresses the formation of biexciton, and thus greatly reduces photocharging. The robustness of these QDs is confirmed by their excellent stability under continuous 1 h electron irradiation in high-resolution transmission electron microscope inspection. It is believed that these results mark an important milestone in realizing nonblinking single photon emission in semiconductor QDs.
高发射率半导体纳米晶体,即所谓的量子点(QDs),在从显示器、生物标记到量子通信和现代安全等各种领域都有应用。尽管量子点的集合已经显示出非常高的光致发光量子产率(PLQYs),并已广泛应用于当前的光电子产品中,但在单量子点水平上表现出高吸收截面、高发射强度,以及最重要的非闪烁行为的量子点,长期以来一直是人们所期望的,并且在室温下尚未实现。在这项工作中,展示了基于红外发射的MAPbI卤化物钙钛矿量子点。这些量子点不仅在集合水平上显示出约100%的PLQY,而且令人惊讶的是,在单量子点水平上,显示出高达1.80×10 cm的超大吸收截面和具有95.3%的高单光子纯度的非闪烁单光子发射,这是一种在室温下运行的所有类型量子发射器中极为罕见的独特特性。深入分析表明,在MAPbI量子点中既未观察到三重激子形成,也未观察到带边载流子俘获,从而抑制了强度闪烁和寿命闪烁。光通量依赖的瞬态吸收测量表明,这些钙钛矿量子点中不闪烁行为和高单光子纯度的共存源于显著的排斥性激子 - 激子相互作用,这种相互作用抑制了双激子的形成,从而大大减少了光充电。这些量子点在高分辨率透射电子显微镜检查中连续1小时电子辐照下的出色稳定性证实了它们的稳健性。相信这些结果标志着在实现半导体量子点中的非闪烁单光子发射方面的一个重要里程碑。