Matrix-induced defects and molecular doping in the afterglow of SiO2 microparticles

Xue Chen, Mengfen Che, Weidong Xu, Zhongbin Wu, Yung Doug Suh, Suli Wu, Xiaowang Liu () and Wei Huang ()
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Xue Chen: Northwestern Polytechnical University
Mengfen Che: Northwestern Polytechnical University
Weidong Xu: Northwestern Polytechnical University
Zhongbin Wu: Northwestern Polytechnical University
Yung Doug Suh: Department of Chemistry and School of Energy and Chemical Engineering UNIST
Suli Wu: Dalian University of Technology
Xiaowang Liu: Northwestern Polytechnical University
Wei Huang: Northwestern Polytechnical University

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract A deep understanding of how the host matrix influences the afterglow properties of molecule dopants is crucial for designing advanced afterglow materials. Despite its appeal, the impact of defects on the afterglow performance in molecule-doped SiO2 matrices has remained largely unexplored. Herein, we detail the synthesis of monodisperse SiO2 microparticles by hydrothermally doping molecules, such as 4-phenylpyridine, 4,4’-bipyridine, and 1,4-bis(pyrid-4-yl)benzene. Our results demonstrate that hydrothermal reactions induce not only the formation of emissive defects in the SiO2 matrix but also enable molecule doping through SiO2 pseudomorphic transformation. Optical analyses reveal a remarkable afterglow activation of doped molecules, driven by a synergistic interplay of hydrogen bonding and physical fixation. Specifically, 4-phenylpyridine doping leads to an impressive 227- and 271-fold enhancement in fluorescence and afterglow, respectively, and an extraordinary 3711-fold enhancement in the afterglow lifetime of the resulting SiO2 MPs. We also document hybrid states involving molecule dopants and SiO2 defects, explaining energy transfer from molecule dopants to defects in both singlet and triplet states. The robust achievement of molecule doping provides flexibility to tailor excitation-dependent afterglow attributes while preserving angle-dependent structural colors, facilitating the creation of diverse building blocks for multiscale optical platforms for afterglow modulation and information encoding.

Date: 2024
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DOI: 10.1038/s41467-024-51591-4

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