{"title":"Room-temperature synthesis of triple-cation green perovskite quantum dots for optoelectronic applications†","authors":"Jean-Sébastien Bénas, Fang-Cheng Liang, Yu-Hang Huang, Fu-Chieh Liu, Chun-Hsien Ou, Ryosuke Oikawa, Ryota Kobayashi, Shoki Mizoguchi, Yuna Igarashi, Takayuki Chiba, Junji Kido and Chi-Ching Kuo","doi":"10.1039/D4MH01270D","DOIUrl":null,"url":null,"abstract":"<p >The development of multi-cation perovskite quantum dots (PQDs) is limited by the low availability of fitting A-site cations due to the unsuitable radii of a large gamut of amine cations. The impact of oversized or undersized cations on the perovskite structure is detrimental to the structural stabilization and electroluminescence efficiency of the PQDs. Researchers are actively seeking suitable-sized cations to mitigate perovskite defect formation and optimize charge carrier confinement within the PQDs. In contrast to cesium (Cs) or formamidine (FA), which are exposed to degradation pathways, guanidinium (GA)-doping has been to provide a suitable radius and the lack a dipole moment. The triple nitrogen functionality of GA enables it to passivate both the PbBr<small><sub>6</sub></small> octahedra and surface defects through vacant A-sites and entropically stabilize the perovskite. Furthermore, the insertion of GA into the PQD lattice is enthalpically facilitated by the presence and arrangement of smaller Cs and Br atoms. Herein, we have synthesized a Cs–FA PQD reference into which GA is doped <em>via</em> two chemical routes. Our triple-cation system exhibits substantially improved optical properties and was applied for the fabrication of a PeLED device. The optimized triple-cation PQDs-based PeLED device exhibited an external quantum efficiency of 5.87% and a luminescence of 13726 cd m<small><sup>−2</sup></small>.</p>","PeriodicalId":87,"journal":{"name":"Materials Horizons","volume":" 4","pages":" 1334-1345"},"PeriodicalIF":10.7000,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Materials Horizons","FirstCategoryId":"88","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2025/mh/d4mh01270d","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
The development of multi-cation perovskite quantum dots (PQDs) is limited by the low availability of fitting A-site cations due to the unsuitable radii of a large gamut of amine cations. The impact of oversized or undersized cations on the perovskite structure is detrimental to the structural stabilization and electroluminescence efficiency of the PQDs. Researchers are actively seeking suitable-sized cations to mitigate perovskite defect formation and optimize charge carrier confinement within the PQDs. In contrast to cesium (Cs) or formamidine (FA), which are exposed to degradation pathways, guanidinium (GA)-doping has been to provide a suitable radius and the lack a dipole moment. The triple nitrogen functionality of GA enables it to passivate both the PbBr6 octahedra and surface defects through vacant A-sites and entropically stabilize the perovskite. Furthermore, the insertion of GA into the PQD lattice is enthalpically facilitated by the presence and arrangement of smaller Cs and Br atoms. Herein, we have synthesized a Cs–FA PQD reference into which GA is doped via two chemical routes. Our triple-cation system exhibits substantially improved optical properties and was applied for the fabrication of a PeLED device. The optimized triple-cation PQDs-based PeLED device exhibited an external quantum efficiency of 5.87% and a luminescence of 13726 cd m−2.
多阳离子钙钛矿量子点(PQDs)的发展受到a位阳离子的低可用性的限制,因为大范围胺离子的半径不合适。过大或过小的阳离子对钙钛矿结构的影响对pqd的结构稳定性和电致发光效率都是不利的。研究人员正在积极寻找合适尺寸的阳离子,以减轻钙钛矿缺陷的形成,并优化pqd内的载流子限制。与暴露于降解途径的铯(Cs)或甲脒(FA)相比,胍(GA)掺杂提供了合适的半径和缺乏偶极矩。GA的三氮官能团使其能够通过空a位钝化PbBr6八面体和表面缺陷,并使钙钛矿的熵稳定。此外,更小的Cs和Br原子的存在和排列在焓上促进了GA插入PQD晶格。在此,我们合成了一个Cs-FA PQD参考,其中GA通过两种化学途径掺杂。我们的三阳离子体系表现出显著改善的光学性能,并应用于PeLED器件的制造。优化后的基于三阳离子pqds的PeLED器件外量子效率为5.87%,发光强度为13726 cd m-2。