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通过多重限制和磷光辅助能量转移实现热增强和长寿命红色热活化延迟荧光碳点

Thermally Enhanced and Long Lifetime Red TADF Carbon Dots via Multi-Confinement and Phosphorescence Assisted Energy Transfer.

作者信息

Lou Qing, Chen Niu, Zhu Jinyang, Liu Kaikai, Li Chao, Zhu Yongsheng, Xu Wen, Chen Xu, Song Zhijiang, Liang Changhao, Shan Chong-Xin, Hu Junhua

机构信息

State Centre for International Cooperation on Designer Low-Carbon & Environmental Materials, School of Materials Science and Engineering, Zhengzhou University, Zhengzhou, 450001, P. R. China.

Key Laboratory of Material Physics, Ministry of Education, School of Physics and Microelectronics, Zhengzhou University, Zhengzhou, 450052, P. R. China.

出版信息

Adv Mater. 2023 May;35(20):e2211858. doi: 10.1002/adma.202211858. Epub 2023 Mar 31.

Abstract

Thermally activated delayed fluorescence (TADF) materials, which can harvest both singlet and triplet excitons for high-efficiency emission, have attracted widespread concern for their enormous applications. Nevertheless, luminescence thermal quenching severely limits the efficiency and operating stability in TADF materials and devices at high temperature. Herein, a surface engineering strategy is adopted to obtain unique carbon dots (CDs)-based thermally enhanced TADF materials with ≈250% enhancement from 273 to 343 K via incorporating seed CDs into ionic crystal network. The rigid crystal network can simultaneously boost reverse intersystem crossing process via enhancing spin-orbit coupling between singlet and triplet states and suppressing non-radiative transition rate, contributing to the thermally enhanced TADF character. Benefiting from efficient energy transfer from triplet states of phosphorescence center to singlet states of CDs, TADF emission at ≈600 nm in CDs displays a long lifetime up to 109.6 ms, outperforming other red organic TADF materials. Thanks to variable decay rates of the delayed emission centers, time and temperature-dependent delayed emission color has been first realized in CDs-based delayed emission materials. The CDs with thermally enhanced and time-/temperature-dependent emission in one material system can offer new opportunities in information protection and processing.

摘要

热激活延迟荧光(TADF)材料能够捕获单线态和三线态激子以实现高效发光,因其巨大的应用潜力而备受广泛关注。然而,发光热猝灭严重限制了TADF材料及器件在高温下的效率和工作稳定性。在此,通过将种子碳点(CDs)掺入离子晶体网络,采用表面工程策略获得了独特的基于碳点的热增强TADF材料,在273至343 K范围内增强约250%。刚性晶体网络可通过增强单线态和三线态之间的自旋 - 轨道耦合以及抑制非辐射跃迁速率,同时促进反向系间窜越过程,从而赋予热增强TADF特性。得益于从磷光中心的三线态到碳点单线态的高效能量转移,碳点中约600 nm处的TADF发射显示出长达109.6 ms的长寿命,优于其他红色有机TADF材料。由于延迟发射中心的衰减速率可变,首次在基于碳点的延迟发射材料中实现了时间和温度相关的延迟发射颜色。在一个材料体系中具有热增强以及时间/温度相关发射的碳点可为信息保护和处理提供新机遇。

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