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Broadening Phosphor-Converted Light-Emitting Diode Emission: Controlling Disorder

  • Chih-Yu Chang
    Chih-Yu Chang
    Department of Chemistry, National Taiwan University, Taipei 106, Taiwan
  • Natalia Majewska
    Natalia Majewska
    Institute of Experimental Physics, Faculty of Mathematics, Physics and Informatics, University of Gdansk, Wita Stwosza 57, 80-308 Gdansk, Poland
  • Kuan-Chun Chen
    Kuan-Chun Chen
    Department of Chemistry, National Taiwan University, Taipei 106, Taiwan
  • Wen-Tse Huang
    Wen-Tse Huang
    Department of Chemistry, National Taiwan University, Taipei 106, Taiwan
  • Tadeusz Leśniewski
    Tadeusz Leśniewski
    Institute of Experimental Physics, Faculty of Mathematics, Physics and Informatics, University of Gdansk, Wita Stwosza 57, 80-308 Gdansk, Poland
  • 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
  • Sławomir M. Kaczmarek
    Sławomir 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
  • Wei Kong Pang
    Wei Kong Pang
    Institute for Superconducting and Electronic Materials, University of Wollongong, Squires Way, North Wollongong, New South Wales 2522, Australia
  • 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
  • Ding-Hua Cherng
    Ding-Hua Cherng
    Everlight Electronics Co., Ltd., New Taipei City 238, Taiwan
  • Kuang-Mao Lu
    Kuang-Mao Lu
    Everlight Electronics Co., Ltd., New Taipei City 238, Taiwan
    More by Kuang-Mao Lu
  • Sebastian Mahlik*
    Sebastian Mahlik
    Institute of Experimental Physics, Faculty of Mathematics, Physics and Informatics, University of Gdansk, Wita Stwosza 57, 80-308 Gdansk, Poland
    *Email: [email protected]
  • , and 
  • Ru-Shi Liu*
    Ru-Shi Liu
    Department of Chemistry, National Taiwan University, Taipei 106, Taiwan
    *Email: [email protected]
    More by Ru-Shi Liu
Cite this: Chem. Mater. 2022, 34, 22, 10190–10199
Publication Date (Web):November 7, 2022
https://doi.org/10.1021/acs.chemmater.2c03045
Copyright © 2022 American Chemical Society

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    Abstract

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    Near-infrared (NIR) phosphor-converted light-emitting diodes (pc-LEDs) are a highly efficient perspective NIR light source, with application hindered by a narrow emission band. In this work, we broaden the emission of a new series of NIR phosphors by controlling crystal structure disorder through cation cosubstitution. By substituting Ga3+ with (Al0.68In0.32)3+, we create a Ga2–x(Al0.68In0.32)xO3:Cr3+ phosphor series in which the average crystal size is maintained, while cation disorder varies. The increased deviation of the cation radii in the substitution leads to increased electron–phonon coupling, with a resulting emission spectrum covering the 650–1000 nm range with a 30% increase in the emission full width at half-maximum (FWHM) and a relatively high internal quantum efficiency of ∼80%. A transition from the β phase to the α phase, which differs in structure from the undoped parent, is created by the application of high pressure and possesses ultra-broad-band emission and an FWHM of ∼190 nm. This work shows that the emission bandwidth can be controlled through disorder and its influence on the Stokes shift, as captured by the effective Huang–Rhys factor.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.chemmater.2c03045.

    • Detailed experimental characterization results; XRD and NPD refinements; X-ray absorption near-edge spectroscopy (XANES); Raman spectroscopy; luminescence measurements; crystal field calculations including pressure-dependent energy diagrams; decay profiles; chemical pressure studies; EPR; and SQUID measurements (PDF)

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    Cited By

    This article is cited by 4 publications.

    1. Chih-Yu Chang, Ming-Hsuan Huang, Kuan-Chun Chen, Wen-Tse Huang, Mikołaj Kamiński, Natalia Majewska, Tomasz Klimczuk, Jia-Hao Chen, Ding-Hua Cherng, Kuang-Mao Lu, Wei Kong Pang, Vanessa K. Peterson, Sebastian Mahlik, Grzegorz Leniec, Ru-Shi Liu. Ultrahigh Quantum Efficiency Near-Infrared-II Emission Achieved by Cr3+ Clusters to Ni2+ Energy Transfer. Chemistry of Materials 2024, 36 (8) , 3941-3948. https://doi.org/10.1021/acs.chemmater.4c00438
    2. Natalia Majewska, Yi-Ting Tsai, Xiang-Yun Zeng, Mu-Huai Fang, Sebastian Mahlik. Advancing Near-Infrared Light Sources: Enhancing Chromium Emission through Cation Substitution in Ultra-Broadband Near-Infrared Phosphors. Chemistry of Materials 2023, 35 (23) , 10228-10237. https://doi.org/10.1021/acs.chemmater.3c02466
    3. Grzegorz Leniec. Electron Paramagnetic Resonance: A Technique to Locate the Nearest Environment of Chromium Luminescent Centers. ACS Applied Optical Materials 2023, 1 (6) , 1114-1121. https://doi.org/10.1021/acsaom.3c00018
    4. Zurong Liao, Chaojie Li, Jiyou Zhong, Yang Li, Weiren Zhao. An efficient and thermally stable near-infrared phosphor derived from the Ln 3 ScInGa 3 O 12 :Cr 3+ (Ln = La, Gd, Y, and Lu) garnet family. Dalton Transactions 2023, 52 (9) , 2853-2862. https://doi.org/10.1039/D2DT04126J

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