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New insight into pyrrolic-N site effect towards the first NIR window absorption of pyrrolic-N-rich carbon dots

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Abstract

Controlled C—N configurations, i.e., pyrrolic-N, pyridinic-N, and graphitic-N, are promising strategies to tailor the carbon dots’ (CDs) optical properties into the first near infrared (NIR) window (650–900 nm), a responsive range for biomedical application. However, a deep understanding of the role of the C—N configuration in the CDs’ properties is still challenging and thought-provoking owing to their complex structure. Here, an underlying pyrrolic-N concentration and position effect on the pyrrolic-N-rich CDs’ absorption was comprehensively elucidated based on the integrated experimental and computational studies. The as-synthesized pyrrolic-N-rich CDs exhibit a first NIR window absorption centered at 650 nm with high photothermal conversion. Pyrrolic-N concentrations from 1.4% to 11.3% and positions (edge and mid-site) were systematically investigated. A mid-site pyrrolic-N was subsequently generated after the pyrrolic-N concentration more than 10%. Edge-site pyrrolic-N induces a frontier orbital hybridization, reducing bandgap energy, while mid-site pyrrolic-N plays a critical role in inducing a first NIR window absorption owing to their high charge transfer. Also, pyrrolic-N-rich CDs inherit a bowl-like topological feature, elevating the CDs’ layer thickness as much as 0.71 nm. This study shed light on the design and optimization of pyrrolic-N on CDs for the first NIR window responsive materials in any biomedical application.

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Acknowledgements

This work was fully supported by the Indonesian Endowment Fund for Education and the Indonesian Science Fund through the International Collaboration RISPRO Funding Program (No. RISPRO/KI/B1/KOM/11/4542/2/2020). F. A. P, R.U, and C. D. D. S would like to thank the Ministry of Fiscal Indonesia Endowment Fund for Education (LPDP) for their master and doctoral scholarship.

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Authors and Affiliations

  1. Department of Physics, Faculty Mathematics and Natural Sciences, Institut Teknologi Bandung, Jalan Ganesha 10, Bandung, West Java, 40132, Indonesia

    Fitri Aulia Permatasari, Reza Umami & Ferry Iskandar

  2. Collaboration Research Center for Advanced Energy Materials, National Research and Innovation Agency — Institut Teknologi Bandung, Jalan Ganesha 10, Bandung, West Java, 40132, Indonesia

    Fitri Aulia Permatasari, Tirta Rona Mayangsari, Fahdzi Muttaqien & Ferry Iskandar

  3. Department of Chemistry, Faculty of Mathematics and Natural Sciences, Institut Teknologi Bandung, Jl. Ganesha 10, Bandung, West Java, 40132, Indonesia

    Citra Deliana Dewi Sundari & Atthar Luqman Ivansyah

  4. Department of Chemistry Education, UIN Sunan Gunung Djati Bandung, Jl. Cimincrang, Bandung, West Java, 40292, Indonesia

    Citra Deliana Dewi Sundari

  5. Department of Chemistry, Universitas Pertamina, Jakarta, 12220, Indonesia

    Tirta Rona Mayangsari

  6. Master Program in Computational Science, Faculty of Mathematics and Natural Sciences, Institut Teknologi Bandung, Jl. Ganesha 10, Bandung, West Java, 40132, Indonesia

    Atthar Luqman Ivansyah & Fahdzi Muttaqien

  7. Instrumentation and Computational Physics Research Group, Faculty of Mathematics and Natural Sciences, Institut Teknologi Bandung, Jl. Ganesha 10, Bandung, 40132, Indonesia

    Fahdzi Muttaqien

  8. Research Center for Nanoscience and Nanotechnology, Institut Teknologi Bandung, Jalan Ganesha 10, Bandung, West Java, 40132, Indonesia

    Fahdzi Muttaqien & Ferry Iskandar

  9. Chemical Engineering Program, Department of Advanced Science and Engineering, Graduate School of Advanced Science and Engineering, Hiroshima University, Higashi-Hiroshima, 739-8527, Japan

    Takashi Ogi

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  1. Fitri Aulia Permatasari
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Permatasari, F.A., Umami, R., Sundari, C.D.D. et al. New insight into pyrrolic-N site effect towards the first NIR window absorption of pyrrolic-N-rich carbon dots. Nano Res. 16, 6001–6009 (2023). https://doi.org/10.1007/s12274-022-5131-7

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