Carbon Dots With Aggregation-Dependent Photoluminescence and Application in Rewritable Water-Jet Printing

Abstract

Carbon dots (CDs) have garnered significant attention for their excellent and versatile optical properties. Nevertheless, the influence of aggregation states on the photophysical properties of CDs has not yet been systematically elucidated. Herein, we present a systematic investigation into the aggregation-dependent photophysical behavior of CDs with a Si-O-Si-encapsulated luminescent carbon core and surface long-chain fatty amines. This study reveals two distinct pathways for emission modulation: (1) achieving concentration-dependent photoluminescence for CDs, spanning from green (λ_em = 527 nm) to deep red (λ_em = 672 nm); and (2) inducing the self-assembly of CDs into size-tunable nano- to micro-scale spherical structures in a poor solvent, which exhibit aggregation-induced emission with a maximum photoluminescence quantum yield of 87.6%. This unique dual-mode aggregation-dependent photoluminescence enables the successful application of CDs in rewritable water‑jet printing, highlighting their strong potential for practical uses.

Keywords

aggregation-induced emission / assembly / carbon dots / concentration-dependent photoluminescence / rewritable water‑jet printing

References

[1] L. Ðorđević, F. Arcudi, M. Cacioppo, and M. Prato, “A Multifunctional Chemical Toolbox to Engineer Carbon Dots for Biomedical and Energy Applications,” Nature Nanotechnology 17 (2022): 112-130.

[2] C. Xia, J. Zhong, X. Han, et al., “The Formation Mechanism of Carbonized Polymer Dots: Crosslinking-Induced Nucleation and Carbonization,” Angewandte Chemie International Edition 63 (2024): e202410519.

[3] G. Ragazzon, A. Cadranel, E. V. Ushakova, et al., “Optical Processes in Carbon Nanocolloids,” Chem 7 (2021): 606-628.

[4] Y. Shi, W. Su, F. Yuan, et al., “Carbon Dots for Electroluminescent Light-Emitting Diodes: Recent Progress and Future Prospects,” Advanced Materials 35 (2023): 2210699.

[5] B. Wang and S. Lu, “The Light of Carbon Dots: From Mechanism to Applications,” Matter 5 (2022): 110-149.

[6] Y. Liu, Z. Huang, X. Wang, et al., “Recent Advances in Highly Luminescent Carbon Dots,” Advanced Functional Materials 35 (2025): 2420587.

[7] A. Döring, E. Ushakova, and A. L. Rogach, “Chiral Carbon Dots: Synthesis, Optical Properties, and Emerging Applications,” Light: Science & Applications 11 (2022): 75.

[8] B. Wang, J. Wang, and S. Lu, “Carbon Dots: Small Materials With Big Impacts on Optoelectronic Devices,” Aggregate 6 (2025): e70212.

[9] H. Ding, T. Xiao, F. Ren, et al., “Carbon-Based Nanodots for Biomedical Applications and Clinical Transformation Prospects,” BMEMat 2 (2024): e12085.

[10] H. Song, Y. Ru, J. Yu, et al., “Carbon Dots: From Fundamentals to Frontier Applications,” Science China Chemistry 69 (2026): 539-618.

[11] H. A. Nguyen, I. Srivastava, D. Pan, and M. Gruebele, “Unraveling the Fluorescence Mechanism of Carbon Dots With Sub-Single-Particle Resolution,” ACS Nano 14 (2020): 6127-6137.

[12] C. Ji, F. Zeng, W. Xu, et al., “Hydrogen Bond-Mediated Self-Assembly of Carbon Dots Enabling Precise Tuning of Particle and Cluster Luminescence for Advanced Optoelectronic Applications,” Advanced Materials 37 (2025): 2414450.

[13] D. Li, Y. Qu, X. Zhang, W. Zheng, A. L. Rogach, and S. Qu, “Supra-(Carbon Dots) With Versatile Morphologies and Promising Optical Properties,” Chemical Engineering Journal 454 (2023): 140069.

[14] W. Xu, F. Zeng, Q. Han, and Z. Peng, “Recent Advancements of Solid-State Emissive Carbon Dots: A Review,” Coordination Chemistry Reviews 498 (2024): 215469.

[15] T. Förster and K. Kasper, “Ein Konzentrationsumschlag der Fluoreszenz,” Zeitschrift Fur Physikalische Chemie 1 (1954): 275-277.

[16] R.-W. Song, C.-L. Shen, G.-S. Zheng, et al., “Supramolecular Aggregation of Carbon Nanodots,” Nano Letters 23 (2023): 11669-11677.

[17] Y. Ru, G. I. N. Waterhouse, and S. Lu, “Aggregation in Carbon Dots,” Aggregate 3 (2022): e296.

[18] L. Ai, H. Wang, B. Wang, S. Liu, H. Song, and S. Lu, “Concentration-Switchable Assembly of Carbon Dots for Circularly Polarized Luminescent Amplification in Chiral Logic Gates and Deep-Red Light-Emitting Diodes,” Advanced Materials 36 (2024): 2410094.

[19] H. Yang, Y. Liu, Z. Guo, et al., “Hydrophobic Carbon Dots With Blue Dispersed Emission and Red Aggregation-Induced Emission,” Nature Communications 10 (2019): 1789.

[20] X. Chen, X. Zhang, L. Xia, H. Wang, Z. Chen, and F. Wu, “One-Step Synthesis of Ultrasmall and Ultrabright Organosilica Nanodots With 100% Photoluminescence Quantum Yield: Long-Term Lysosome Imaging in Living, Fixed, and Permeabilized Cells,” Nano Letters 18 (2018): 1159-1167.

[21] D. W. Boukhvalov, V. Y. Osipov, D. Murzalinov, A. Serikkanov, and H. Bi, “A Comprehensive Model of Carbon Nanodots With 0.21 Nm Lattice Fringes Patterns,” Carbon 225 (2024): 119101.

[22] Y. Zheng, K. Arkin, J. Hao, et al., “Multicolor Carbon Dots Prepared by Single-Factor Control of Graphitization and Surface Oxidation for High-Quality White Light-Emitting Diodes,” Advanced Optical Materials 9 (2021): 2100688.

[23] S. Bhattacharya, R. S. Phatake, S. Nabha Barnea, et al., “Fluorescent Self-Healing Carbon Dot/Polymer Gels,” ACS Nano 13 (2019): 1433-1442.

[24] G. Hu, Y. Wang, S. Zhang, et al., “Rational Synthesis of Silane-Functionalized Carbon Dots With High-Efficiency Full-Color Solid-State Fluorescence for Light Emitting Diodes,” Carbon 203 (2023): 1-10.

[25] Y. Wu, L. Zhao, X. Cao, et al., “Bright and Multicolor Emissive Carbon Dots/Organosilicon Composite for Highly Efficient Tandem Luminescent Solar Concentrators,” Carbon 207 (2023): 77-85.

[26] X. Chen, X. Zhang, and F. Wu, “Ultrasmall Green-Emitting Carbon Nanodots With 80% Photoluminescence Quantum Yield for Lysosome Imaging,” Chinese Chemical Letters 32 (2021): 3048-3052.

[27] F. Yan, H. Zhang, J. Xu, Y. Wu, Y. Zang, and J. Sun, “Color Emission Carbon Dots With Quench-ResixAstant Solid-State Fluorescence for Light-Emitting Diodes,” ACS Sustainable Chemistry & Engineering 9 (2021): 3901-3908.

[28] M. Sun, B. Tian, X. Li, et al., “Carbon Dots With Tunable Excitation-Independent Fluorescence and Organelle-Specific Targeting via Core Graphitization and Surface Groups Engineering,” Chemical Engineering Journal 496 (2024): 153729.

[29] X. Huang, W. Ye, J. Zhuang, et al., “π-Conjugated Structure Enhances the UV Absorption Performance of Carbon Dots and Application in the Design of Light-Colored Sunglasses,” ACS Sustainable Chemistry & Engineering 12 (2024): 10399-10410.

[30] K. M. Chan, D. K. Kölmel, S. Wang, and E. T. Kool, “Color-Change Photoswitching of an Alkynylpyrene Excimer Dye,” Angewandte Chemie International Edition 56 (2017): 6497-6501.

[31] S. Zhao, H. Wang, J. He, et al., “Developing Dual-State Ultra-Efficient Emissive Carbon Dots as Internal and External Artificial Antenna of Chloroplasts to Enhance Plant-Photosynthesis,” Aggregate 5 (2024): e625.

[32] D. Li, D. Han, S.-N. Qu, et al., “Supra-(Carbon Nanodots) With a Strong Visible to Near-Infrared Absorption Band and Efficient Photothermal Conversion,” Light: Science and Applications 5 (2016): e16120.

[33] L. Dou, H. Zheng, H. Xiong, S. Fu, C. Wang, and D. Li, “π-Bridged Dimer Strategy of Aggregation-Induced Emission Molecules to Achieve Very Strong Absorption Ability,” Aggregate 6 (2025): e70068.

[34] H. B. Rodríguez, M. Mirenda, M. G. Lagorio, and E. San Román, “Photophysics at Unusually High Dye Concentrations,” Accounts of Chemical Research 52 (2019): 110-118.

[35] J. Zhang, L. Hu, K. Zhang, et al., “How to Manipulate Through-Space Conjugation and Clusteroluminescence of Simple AIEgens With Isolated Phenyl Rings,” Journal of the American Chemical Society 143 (2021): 9565-9574.

[36] Y. Zhao, L. Xu, Y. He, Z. Feng, W. Feng, and H. Yan, “Nonconventional Aggregation-Induced Emission Polysiloxanes: Structures, Characteristics, and Applications,” Aggregate 5 (2024): e471.

[37] P. P. N. Syamala, B. Soberats, D. Görl, S. Gekle, and F. Würthner, “Thermodynamic Insights Into the Entropically Driven Self-Assembly of Amphiphilic Dyes in Water,” Chemical Science 10 (2019): 9358-9366.

[38] G. Xi, L. Sheng, J. Du, et al., “Water Assisted Biomimetic Synergistic Process and Its Application in Water-Jet Rewritable Paper,” Nature Communications 9 (2018): 4819.

[39] L. Sheng, M. Li, S. Zhu, et al., “Hydrochromic Molecular Switches for Water-Jet Rewritable Paper,” Nature Communications 5 (2014): 3044.

[40] J. Mei, N. L. C. Leung, R. T. K. Kwok, J. W. Y. Lam, and B. Z. Tang, “Aggregation-Induced Emission: Together We Shine, United We Soar!,” Chemical Reviews 115 (2015): 11718-11940.

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2026 The Author(s). Aggregate published by SCUT, AIEI, and John Wiley & Sons Australia, Ltd.