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Electronic State Engineering in Perovskite-Cerium-Composite Nanocrystals toward Enhanced Triplet Annihilation Upconversion
Advanced Science ( IF 14.3 ) Pub Date : 2023-10-23 , DOI: 10.1002/advs.202305069
Nan Gong 1 , Runchen Lai 1 , Shiyu Xing 1 , ZhengZheng Liu 2 , Junyao Mo 1 , Tao Man 1 , Zicheng Li 1 , Dawei Di 1 , Juan Du 2 , Dezhi Tan 3 , Xiaofeng Liu 4 , Jianrong Qiu 1 , Beibei Xu 1
Affiliation  

Wavelength conversion based on hybrid inorganic–organic sensitized triplet–triplet annihilation upconversion (TTA-UC) is promising for applications such as photovoltaics, light-emitting-diodes, photocatalysis, additive manufacturing, and bioimaging. The efficiency of TTA-UC depends on the population of triplet excitons involved in triplet energy transfer (TET), the driving force in TET, and the coupling strength between the donor and acceptor. Consequently, achieving highly efficient TTA-UC necessitates the precise control of the electronic states of inorganic donors. However, conventional covalently bonded nanocrystals (NCs) face significant challenges in this regard. Herein, a novel strategy to exert control over electronic states is proposed, thereby enhancing TET and TTA-UC by incorporating ionic-bonded CsPbBr3 and lanthanide Ce3+ ions into composite NCs. These composite-NCs exhibit high photoluminescence quantum yield, extended single-exciton lifetime, quantum confinement, and uplifted energy levels. This engineering strategy of electronic states engendered a comprehensive impact, augmenting the population of triplet excitons participating in the TET process, enhancing coupling strength and the driving force, ultimately leading to an unconventional, dopant concentration-dependent nonlinear enhancement of UC efficiency. This work not only advances fundamental understanding of hybrid TTA-UC but also opens a door for the creation of other ionic-bonded composite NCs with tunable functionalities, promising innovations for next-generation optoelectronic applications.

中文翻译:


钙钛矿-铈复合纳米晶体中的电子态工程增强三重态湮没上转换



基于混合无机-有机敏化三重态-三重态湮没上转换(TTA-UC)的波长转换在光伏、发光二极管、光催化、增材制造和生物成像等应用中具有广阔的前景。 TTA-UC的效率取决于参与三重态能量转移(TET)的三重态激子的数量、TET的驱动力以及供体和受体之间的耦合强度。因此,实现高效 TTA-UC 需要精确控制无机供体的电子态。然而,传统的共价键合纳米晶体(NC)在这方面面临着重大挑战。在此,提出了一种对电子态进行控制的新策略,从而通过将离子键合的CsPbBr 3和镧系元素Ce 3+离子合并到复合NC中来增强TET和TTA-UC。这些复合NC表现出高光致发光量子产率、延长的单激子寿命、量子限制提高的能级。这种电子态的工程策略产生了全面的影响,增加了参与TET过程的三重态激子的数量,增强了耦合强度和驱动力,最终导致非常规的、掺杂剂浓度依赖性的非线性UC效率的增强。这项工作不仅增进了对混合 TTA-UC 的基本理解,而且还为创建其他具有可调功能的离子键合复合 NC 打开了大门,有望为下一代光电应用带来创新。
更新日期:2023-10-23
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