Amide (n, π*) Transitions Enabled Clusteroluminescence in Solid‐State Carbon Dots

Author:

Li Hui‐Jun12,Chen Yanlu1,Wang Hao1,Wang Huan1,Liao Qiaobo1,Han Sancan1,Li Ying1,Wang Ding1,Li Guisheng1,Deng Yonghui13ORCID

Affiliation:

1. School of Materials and Chemistry University of Shanghai for Science and Technology Shanghai 200093 China

2. State Key Lab of Transducer Technology Shanghai Institute of Microsystem and Information Technology Chinese Academy of Sciences Shanghai 200050 China

3. Department of Chemistry State Key Laboratory of Molecular Engineering of Polymers Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials iChEM Fudan University Shanghai 200433 China

Abstract

AbstractCarbon dots (CDs) demonstrate great superiority in optoelectronic devices due to their tunable emission and photobleaching resistance properties. Although the fluorescence of CDs in solution has been extensively studied, their solid‐state fluorescence (SSF) mechanism still remains largely unexplored experimentally. Herein, solid‐state fluorescent CDs with unique clusteroluminescence (CL) generated from clusterization‐triggered emission are designed based on condensation between precursors with carboxyl and amino groups. The CDs demonstrate obvious concentration‐dependent fluorescence and quench‐resistant SSF, which is attributed to the activation of amide (n, π*) transition by the clusterization process. This sub‐luminophore is non‐luminescent at long wavelengths in isolated state, while it induces photoluminescence redshift via through‐space interaction in aggregated state. Besides, the SSF of CDs can be tuned from quenched to quenching‐resistant emission through amide formation, and the dominant fluorescent center of CDs solids is switchable from surface to edge state through amide passivation. Based on their long‐wavelength CL feature, high‐purity red light‐emitting diode devices exhibiting 656‐nm warm light are fabricated with the Commission Internationale de l´Eclairage (CIE) coordinates of (0.66, 0.34) and unchanged wavelength under different driving currents. These findings provide novel insights into the SSF mechanism of CDs and a universal strategy to construct fluorescent materials with tailored properties.

Funder

National Natural Science Foundation of China

Science and Technology Commission of Shanghai Municipality

Publisher

Wiley

Subject

Electrochemistry,Condensed Matter Physics,Biomaterials,Electronic, Optical and Magnetic Materials

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