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氘化诱导碳点能级结构重构以增强光致发光

Deuteration-Induced Energy Level Structure Reconstruction of Carbon Dots for Enhancing Photoluminescence.

作者信息

Yao Zimin, Wen Xiaokun, Hong Xia, Tao Ran, Yin Feifei, Cao Shuo, Yan Jiayi, Wang Kexin, Wang Jiwei

机构信息

College of Physics, Liaoning University, Shenyang, 110036, China.

Key Laboratory of UV-Emitting Materials and Technology (Northeast Normal University), Ministry of Education, Changchun, 130024, China.

出版信息

Adv Sci (Weinh). 2024 Aug;11(29):e2308523. doi: 10.1002/advs.202308523. Epub 2024 May 30.

Abstract

Constrained by a limited understanding of the structure and luminescence mechanisms of carbon dots (CDs), achieving precise enhancement of their photoluminescence (PL) performance without altering the emission wavelength and color remains a challenge. In this work, a deuterated CD is first achieved by simply replacing the reaction solvent from HO to DO. The substitution of D atoms for H atoms is not limited on the surface but also within the internal structure of CDs. Deuteration affects the formation of the π-conjugated network structure by altering the content of sp carbon and sp carbon, ultimately inducing a reconstruction for energy level structure of CDs. Both the intrinsic state and surface state emission, including quantum yield, emission intensity and lifetime, are significantly enhanced after deuteration. It benefits from the reduction in non-radiative transitions, since the lowered vibrational frequencies of D atoms and optimized local energy level distribution in CDs structure. The deuterated CDs are applied in the fabrication of white-light-emitting diodes to show their application potential. This work provides a highly versatile route for improving and controlling photoluminescence performance of CDs and has opportunities to guide the development of CDs for practical applications.

摘要

由于对碳点(CDs)的结构和发光机制了解有限,在不改变发射波长和颜色的情况下实现其光致发光(PL)性能的精确增强仍然是一个挑战。在这项工作中,首先通过简单地将反应溶剂从H₂O替换为D₂O来制备氘代碳点。D原子取代H原子不仅发生在碳点表面,也发生在其内部结构中。氘代通过改变sp²碳和sp³碳的含量影响π共轭网络结构的形成,最终导致碳点能级结构的重构。氘代后,包括量子产率、发射强度和寿命在内的本征态和表面态发射均显著增强。这得益于非辐射跃迁的减少,因为D原子的振动频率降低以及碳点结构中局部能级分布的优化。氘代碳点被应用于白光发光二极管的制造以展示其应用潜力。这项工作为改善和控制碳点的光致发光性能提供了一条高度通用的途径,并有机会指导碳点在实际应用中的发展。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a39c/11304250/6ca6bbf56f12/ADVS-11-2308523-g006.jpg

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