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Chromium Ion Pair Luminescence: A Strategy in Broadband Near-Infrared Light-Emitting Diode Design

  • Veeramani Rajendran
    Veeramani Rajendran
    Department of Chemistry, National Taiwan University, Taipei 106, Taiwan
    Department of Mechanical Engineering and Graduate Institute of Manufacturing Technology, National Taipei University of Technology, Taipei 106, Taiwan
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    Orcidhttps://orcid.org/0000-0003-1479-8829
  • , 
  • Mu-Huai Fang
    Mu-Huai Fang
    Department of Chemistry, National Taiwan University, Taipei 106, Taiwan
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    Orcidhttps://orcid.org/0000-0003-1475-0200
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  • Wen-Tse Huang
    Wen-Tse Huang
    Department of Chemistry, National Taiwan University, Taipei 106, Taiwan
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  • Natalia Majewska
    Natalia Majewska
    Institute of Experimental Physics, Faculty of Mathematics, Physics and Informatics, University of Gdańsk, Wita Stwosza 57, 80-308 Gdańsk, Poland
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    Orcidhttps://orcid.org/0000-0002-1933-0355
  • , 
  • Tadeusz Lesniewski
    Tadeusz Lesniewski
    Institute of Experimental Physics, Faculty of Mathematics, Physics and Informatics, University of Gdańsk, Wita Stwosza 57, 80-308 Gdańsk, Poland
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  • , 
  • Sebastian Mahlik
    Sebastian Mahlik
    Institute of Experimental Physics, Faculty of Mathematics, Physics and Informatics, University of Gdańsk, Wita Stwosza 57, 80-308 Gdańsk, Poland
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    Orcidhttps://orcid.org/0000-0002-9514-049X
  • , 
  • Grzegorz Leniec
    Grzegorz Leniec
    Department of Technical Physics, Faculty of Mechanical Engineering and Mechatronics, West Pomeranian University of Technology Szczecin, al. Piastow 48, 70-311 Szczecin, Poland
    More by Grzegorz Leniec
  • , 
  • Slawomir M. Kaczmarek
    Slawomir M. Kaczmarek
    Department of Technical Physics, Faculty of Mechanical Engineering and Mechatronics, West Pomeranian University of Technology Szczecin, al. Piastow 48, 70-311 Szczecin, Poland
    More by Slawomir M. Kaczmarek
  • , 
  • Wei Kong Pang
    Wei Kong Pang
    Institute for Superconducting and Electronic Materials, University of Wollongong, Squires Way, North Wollongong, New South Wales 2522, Australia
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    Orcidhttps://orcid.org/0000-0002-5118-3885
  • , 
  • Vanessa K. Peterson
    Vanessa K. Peterson
    Institute for Superconducting and Electronic Materials, University of Wollongong, Squires Way, North Wollongong, New South Wales 2522, Australia
    Australian Centre for Neutron Scattering, Australian Nuclear Science and Technology Organisation, Sydney, New South Wales 2232, Australia
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    Orcidhttps://orcid.org/0000-0002-5442-0591
  • , 
  • Kuang-Mao Lu
    Kuang-Mao Lu
    Everlight Electronics Co., Ltd., New Taipei City 238, Taiwan
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  • , 
  • Ho Chang*
    Ho Chang
    Department of Mechanical Engineering and Graduate Institute of Manufacturing Technology, National Taipei University of Technology, Taipei 106, Taiwan
    *[email protected]
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  • , and 
  • Ru-Shi Liu*
    Ru-Shi Liu
    Department of Chemistry, National Taiwan University, Taipei 106, Taiwan
    *[email protected]
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    Orcidhttps://orcid.org/0000-0002-1291-9052
Cite this: J. Am. Chem. Soc. 2021, 143, 45, 19058–19066
Publication Date (Web):November 4, 2021
https://doi.org/10.1021/jacs.1c08334
Copyright © 2021 American Chemical Society
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    Abstract

    Abstract Image

    Portable near-infrared (NIR) light sources are in high demand for applications in spectroscopy, night vision, bioimaging, and many others. Typical phosphor designs feature isolated Cr3+ ion centers, and it is challenging to design broadband NIR phosphors based on Cr3+–Cr3+ pairs. Here, we explore the solid-solution series SrAl11.88–xGaxO19:0.12Cr3+ (x = 0, 2, 4, 6, 8, 10, and 12) as phosphors featuring Cr3+–Cr3+ pairs and evaluate structure–property relations within the series. We establish the incorporation of Ga within the magentoplumbite-type structure at five distinct crystallographic sites and evaluate the effect of this incorporation on the Cr3+–Cr3+ ion pair proximity. Electron paramagnetic measurements reveal the presence of both isolated Cr3+ and Cr3+–Cr3+ pairs, resulting in NIR luminescence at approximately 650–1050 nm. Unexpectedly, the origin of broadband NIR luminescence with a peak within the range 740–820 nm is related to the Cr3+–Cr3+ ion pair. We demonstrate the application of the SrAl5.88Ga6O19:0.12Cr3+ phosphor, which possesses an internal quantum efficiency of ∼85%, a radiant flux of ∼95 mW, and zero thermal quenching up to 500 K. This work provides a further understanding of spectral shifts in phosphor solid solutions and in particular the application of the magentoplumbites as promising next-generation NIR phosphor host systems.

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    • Details of characterization, Rietveld fit profiles along with refined structural parameters, pressure-dependent decay profiles and calculated decay time, temperature-dependent emission spectra of x = 4, 6, and 8 samples, and temperature-dependent decay profiles (PDF)

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