Rare-Earth-Metal-Free Solid-State Fluorescent Carbonized-Polymer Microspheres for Unclonable Anti-Counterfeit Whispering-Gallery Emissions from Red to Near-Infrared Wavelengths

Barun Kumar Barman; Hiroyuki Yamada; Keisuke Watanabe; Kenzo Deguchi; Shinobu Ohki; Kenjiro Hashi; Atsushi Goto; Tadaaki Nagao

doi:10.48505/nims.4952

Article Rare-Earth-Metal-Free Solid-State Fluorescent Carbonized-Polymer Microspheres for Unclonable Anti-Counterfeit Whispering-Gallery Emissions from Red to Near-Infrared Wavelengths

Barun Kumar Barman (Research Center for Materials Nanoarchitectonics (MANA)/Quantum Materials Field/Photonics Nano Engineering Group, National Institute for Materials Science) ; Hiroyuki Yamada (Research Center for Materials Nanoarchitectonics (MANA)/Quantum Materials Field/Photonics Nano Engineering Group, National Institute for Materials Science) ; Keisuke Watanabe (Research Center for Materials Nanoarchitectonics (MANA)/Quantum Materials Field/Photonics Nano Engineering Group, National Institute for Materials Science) ; Kenzo Deguchi (Research Network and Facility Services Division/Materials Fabrication and Analysis Platform/High Magnetic Field Characterization Unit, National Institute for Materials Science) ; Shinobu Ohki (Research Network and Facility Services Division/Materials Fabrication and Analysis Platform/High Magnetic Field Characterization Unit, National Institute for Materials Science) ; Kenjiro Hashi (Center for Basic Research on Materials/Advanced Materials Characterization Field/Solid-State NMR Group, National Institute for Materials Science) ; Atsushi Goto (Center for Basic Research on Materials/Advanced Materials Characterization Field/Solid-State NMR Group, National Institute for Materials Science) ; Tadaaki Nagao (Research Center for Materials Nanoarchitectonics (MANA)/Quantum Materials Field/Photonics Nano Engineering Group, National Institute for Materials Science)

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Barun Kumar Barman, Hiroyuki Yamada, Keisuke Watanabe, Kenzo Deguchi, Shinobu Ohki, Kenjiro Hashi, Atsushi Goto, Tadaaki Nagao. Rare-Earth-Metal-Free Solid-State Fluorescent Carbonized-Polymer Microspheres for Unclonable Anti-Counterfeit Whispering-Gallery Emissions from Red to Near-Infrared Wavelengths. Advanced Science. 2024, 11 (30), 2400693. https://doi.org/10.48505/nims.4952

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Colloidal carbon dots (CDs) have garnered much attention as metal-free photoluminescent nanomaterials, yet creation of solid-state fluorescent (SSF) materials emitting in the deep red (DR) to near-infrared (NIR) range poses a significant challenge with practical implications. To address this challenge and to engineer photonic functionalities, a micro-resonator architecture is developed using carbonized polymer microspheres (CPMs), evolved from conventional colloidal nanodots. Gram-scale production of CPMs utilizes controlled microscopic phase separation facilitated by natural peptide cross-linking during hydrothermal processing. The resulting microstructure effectively suppresses aggregation-induced quenching (AIQ), enabling strong solid-state light emission. Both experimental and theoretical analysis support a role for extended π conjugated polycyclic aromatic hydrocarbons (PAHs) trapped within these microstructures, which exhibit a progressive red shift in light absorption/emission toward the NIR range. Moreover, the highly spherical shape of CPMs endows them with innate photonic functionalities in combination with their intrinsic CD-based attributes. Harnessing their excitation wavelength-dependent photoluminescent (PL) property, a single CPM exhibits whispering-gallery modes (WGMs) that are emission-tunable from the DR to the NIR. This type of newly developed microresonator can serve as, for example, unclonable anti-counterfeiting labels. This innovative cross-cutting approach, combining photonics and chemistry, offers robust, bottom-up, built-in photonic functionality with diverse NIR applications.

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