Decisive role of organic fluorophore and surface defect state in the photoluminescence of carbon quantum dots

IF 3.5 2区 物理与天体物理 Q2 PHYSICS, APPLIED Applied Physics Letters Pub Date : 2024-11-26 DOI:10.1063/5.0237147
Chao Jiang, Xifang Chen, Xiaowen Zhang, Yue Zhou, Hongwen Han, Jiangang Yao, Li Liu, Zao Yi
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Abstract

Carbon quantum dots (CQDs) hold significant promise for applications in biological imaging, sensing, and optoelectronic devices owing to their superior photostability and low toxicity. Nevertheless, the elucidation of their photoluminescence mechanism remains an open question, necessitating further comprehensive investigation. In this Letter, CQDs exhibiting ultraviolet (UV) and white fluorescence were isolated through silica gel column chromatography separation of the crude product obtained from a one-step solvothermal synthesis. CQDs with different luminescent properties exhibit the same crystal structure and similar particle size distributions. Both CQDs exhibit orthorhombic structure where C60/C70 molecules are located at lattice points, having average particle sizes of 2.71 and 2.98 nm, respectively. Consequently, the luminescent properties of the synthesized CQDs are predominantly governed by their surface structure. The results of microstructure characterization and spectroscopic analysis demonstrate that the UV emission originates from the C(=O)OH and C–O–C related luminescent moieties within organic fluorophores, and the blue emission band is attributed to defect states related to surface group C–O–C, while the green/yellow emission arises from C(=O)O related surface defect levels. These observations have gained a profound understanding of the luminescent genesis of CQDs, broadened the luminescence coverage wavelength range of CQDs, and enriched the family of CQDs materials.
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有机荧光团和表面缺陷态在碳量子点光致发光中的决定性作用
碳量子点(CQDs)具有优异的光稳定性和低毒性,因此在生物成像、传感和光电设备中的应用前景十分广阔。然而,如何阐明其光致发光机制仍是一个未决问题,需要进一步的全面研究。在这封信中,通过硅胶柱色谱分离一步溶热合成得到的粗产物,分离出了具有紫外(UV)和白色荧光的 CQDs。具有不同发光特性的 CQDs 具有相同的晶体结构和相似的粒度分布。两种 CQD 都呈现出正交菱形结构,其中 C60/C70 分子位于晶格点上,平均粒径分别为 2.71 纳米和 2.98 纳米。因此,合成的 CQDs 的发光特性主要受其表面结构的影响。微观结构表征和光谱分析结果表明,紫外发射源于有机荧光团中与 C(=O)OH 和 C-O-C 相关的发光分子,蓝色发射带归因于与表面基团 C-O-C 相关的缺陷态,而绿色/黄色发射源于与 C(=O)O 相关的表面缺陷水平。这些观察结果深刻揭示了 CQDs 的发光成因,拓宽了 CQDs 的发光覆盖波长范围,丰富了 CQDs 材料家族。
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来源期刊
Applied Physics Letters
Applied Physics Letters 物理-物理:应用
CiteScore
6.40
自引率
10.00%
发文量
1821
审稿时长
1.6 months
期刊介绍: Applied Physics Letters (APL) features concise, up-to-date reports on significant new findings in applied physics. Emphasizing rapid dissemination of key data and new physical insights, APL offers prompt publication of new experimental and theoretical papers reporting applications of physics phenomena to all branches of science, engineering, and modern technology. In addition to regular articles, the journal also publishes invited Fast Track, Perspectives, and in-depth Editorials which report on cutting-edge areas in applied physics. APL Perspectives are forward-looking invited letters which highlight recent developments or discoveries. Emphasis is placed on very recent developments, potentially disruptive technologies, open questions and possible solutions. They also include a mini-roadmap detailing where the community should direct efforts in order for the phenomena to be viable for application and the challenges associated with meeting that performance threshold. Perspectives are characterized by personal viewpoints and opinions of recognized experts in the field. Fast Track articles are invited original research articles that report results that are particularly novel and important or provide a significant advancement in an emerging field. Because of the urgency and scientific importance of the work, the peer review process is accelerated. If, during the review process, it becomes apparent that the paper does not meet the Fast Track criterion, it is returned to a normal track.
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