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Theoretical investigation of fluorescent behavior for p- and n-type atomic-doped graphene quantum dots interacting with Hg (0)

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Abstract

Graphene quantum dots (GQDs) with heteroatomic do** have emerged as a new type of fluorescent probing nanomaterials. The critical point of the application is the precise recognition of the controlling mechanism for varied fluorescent behavior. Herein, density functional theory simulation was performed to investigate the fluorescent behavior of p- and n-type heteroatomic edge-doped GQDs. The n-type (nitrogen)-doped GQDs generally have not shown an obvious fluorescent change with the Hg atom adsorption. However, the p-type (boron)-doped GQDs show a fluorescence red-shift beyond the visible light spectrum accompanied by a weak oscillator strength. This unique fluorescent quenching suggests that the p-type do** could probably have a probing function for elemental Hg. We also characterize the distinct fluorescent behavior for a series of GQDs with co-atomic pair do**. Natural transitional orbitals were applied to examine the energetic variation and electron–hole pair transition. The different photoluminescent phenomena could be ascribed to the differential orbital interactions between GQDs and Hg with varied charge transfers. Our simulation provides a novel insight into the fluorescent behavior of atomic-doped GQDs, which might be valuable for designing doped GQDs and exploring new optical probing applications.

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Data availability

The data that support the findings of this study are available on request from the corresponding author.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China under Grants 21676136. The computational resources generously provided by High Performance Computing Center of Nan**g Tech University are greatly appreciated.

Funding

National Natural Science Foundation of China, 21676136, **aoning Yang

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Authors and Affiliations

  1. State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nan**g Tech University, Nan**g, 211816, China

    Zhaomin Meng, Zhijun Xu & **aoning Yang

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  1. Zhaomin Meng
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  2. Zhijun Xu
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  3. **aoning Yang
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Contributions

ZM contributed to formal analysis, investigation, data curation, and writing—original draft. ZX contributed to formal analysis and investigation. XY contributed to conceptualization, project administration, investigation, methodology, and writing—original draft.

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Correspondence to **aoning Yang.

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10853_2023_9114_MOESM1_ESM.docx

Supplementary Tables S1-S3 and Figs. S1-S13 include detailed composition and electron distribution of HOMO and LUMO in pristine GQDs, the fluorescent spectra, and NTOs patterns of GQDs with Hg adsorption. (DOCX 14193 KB)

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Meng, Z., Xu, Z. & Yang, X. Theoretical investigation of fluorescent behavior for p- and n-type atomic-doped graphene quantum dots interacting with Hg (0). J Mater Sci 58, 17527–17542 (2023). https://doi.org/10.1007/s10853-023-09114-x

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