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

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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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First published at
Creator
  • Name
    Barun Kumar Barman
    ORCID
    https://orcid.org/0000-0002-9894-1890
    Organization
    National Institute for Materials Science
    Sub organization
    Research Center for Materials Nanoarchitectonics (MANA)/Quantum Materials Field/Photonics Nano Engineering Group
    Role
    author
    Name
    Hiroyuki Yamada
    ORCID
    https://orcid.org/0000-0003-0394-857X
    Organization
    National Institute for Materials Science
    Sub organization
    Research Center for Materials Nanoarchitectonics (MANA)/Quantum Materials Field/Photonics Nano Engineering Group
    Role
    author
    Name
    Keisuke Watanabe
    ORCID
    https://orcid.org/0000-0002-4285-2135
    Organization
    National Institute for Materials Science
    Sub organization
    Research Center for Materials Nanoarchitectonics (MANA)/Quantum Materials Field/Photonics Nano Engineering Group
    Role
    author
    Name
    Kenzo Deguchi
    Organization
    National Institute for Materials Science
    Sub organization
    Research Network and Facility Services Division/Materials Fabrication and Analysis Platform/High Magnetic Field Characterization Unit
    Role
    author
    Name
    Shinobu Ohki
    ORCID
    https://orcid.org/0000-0002-7357-3833
    Organization
    National Institute for Materials Science
    Sub organization
    Research Network and Facility Services Division/Materials Fabrication and Analysis Platform/High Magnetic Field Characterization Unit
    Role
    author
    Name
    Kenjiro Hashi
    ORCID
    https://orcid.org/0000-0002-0320-4768
    Organization
    National Institute for Materials Science
    Sub organization
    Center for Basic Research on Materials/Advanced Materials Characterization Field/Solid-State NMR Group
    Role
    author
    Name
    Atsushi Goto
    ORCID
    https://orcid.org/0000-0002-9472-4098
    Organization
    National Institute for Materials Science
    Sub organization
    Center for Basic Research on Materials/Advanced Materials Characterization Field/Solid-State NMR Group
    Role
    author
    Name
    Tadaaki Nagao
    ORCID
    https://orcid.org/0000-0002-6746-2686
    Organization
    National Institute for Materials Science
    Sub organization
    Research Center for Materials Nanoarchitectonics (MANA)/Quantum Materials Field/Photonics Nano Engineering Group
    Role
    author
Keyword
Resource type
Publisher
Date published
  • 12/06/2024
Rights statement
License description
Journal
  • Title
    Advanced Science
    ISSN
    21983844
    Article number
    2400693
    Volume
    11
    Issue
    30
Manuscript type
  • Accepted manuscript
Language
Funding reference
  • Funder identifier
    24K17589
    Funder name
    JSPS
    Award title
    Chromaticity-adaptive direct white light generation from luminescent carbogenic nanomaterials coupled with nanophotonic cavity

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