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Relation between material structure and photoluminescence properties in yttrium–aluminum borates phosphors

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Abstract

Glassy yttrium and aluminum borate powders (g-YAB) were synthesized by the polymeric precursor method (modified Pechini). We report here a detailed study of the structural, spectroscopic, and optical characterizations of the g-YAB powders, involving several complementary techniques: thermal analysis, X-ray powder diffraction, and electron microscopy combined with IR, nuclear magnetic resonance, and electron paramagnetic resonance spectroscopies. All these results, directly correlated with the photoluminescence (PL) properties of the g-YAB phosphors, allow us to argue that the PL emissions come from large polyaromatic molecules auto-generated from organic precursors and trapped in the glassy network of the g-YAB during thermal treatments. These extended aromatic molecules (seven rings and more corresponding to polycyclic aromatic hydrocarbons) must have been produced during the pyrolysis treatment of the powders, in which a large fraction of the protons was replaced during the calcination process by hydroxyl groups, or other oxygen-containing groups.

Impact statement

Substituting critical materials and the reduction of energy consumption of key functional devices, such as LED lighting, are major concerns in materials chemistry research. In this context, the search for new LED phosphors, without rare earths, has given rise to extensive publications. In particular, defects-related luminescent materials and carboneous luminescent species are very promising, as they exhibit broad emissions in the visible range. Moreover, they are synthesized by soft chemical routes at moderate temperatures. However, the mechanisms involved in their photoluminescence (PL) are poorly understood. We report here on the synthesis and properties of yttrium aluminum borate powders–a new broad-emission phosphor–using the low-cost and versatile polymeric precursor method. We combined structural, chemical, and spectroscopic analyses to link the inorganic matrix structure with the intense PL. The inorganic aluminum borate matrix is amorphous, and its structure evolution is not correlated to that of photoluminescence. Moreover, by coupling spectroscopic results (e.g., PL, EPR) and DFT calculations, we specified the molecular nature of the emitting centers that are polycyclic aromatic hydrocarbons, such as coronene or circumcoronene molecules. Thus, these highly original results are an important step in the understanding and identification of the emitting centers in this new family of promising phosphors.

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Acknowledgments

We thank the French National EPR facilities network (IR RENARD CNRS 3443) for support of EPR experiments in this work.

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Authors and Affiliations

  1. Université Grenoble Alpes, CNRS, Grenoble INP, Institut Néel, 38000, Grenoble, France

    M. Salaün, V. F. Guimaraes, I. Gautier-Luneau & A. Ibanez

  2. PSL Research University, Chimie ParisTech - CNRS, Institut de Recherche de Chimie Paris, 75005, Paris, France

    A. D. Sontakke & B. Viana

  3. Université Grenoble Alpes, CEA, CNRS, IRIG, SyMMES, 38000, Grenoble, France

    V. Maurel & J. M. Mouesca

  4. Laboratoire National Des Champs Magnétiques Intenses, UPR CNRS 3228, Université Grenoble Alpes, 38042, Grenoble, France

    A. L. Barra

  5. CEMHTI, CNRS UPR3079, Université Orléans, 45071, Orléans, France

    V. Montouillout

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  1. M. Salaün
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  2. A. D. Sontakke
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  3. V. Maurel
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  4. J. M. Mouesca
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  9. I. Gautier-Luneau
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Salaün, M., Sontakke, A.D., Maurel, V. et al. Relation between material structure and photoluminescence properties in yttrium–aluminum borates phosphors. MRS Bulletin 47, 231–242 (2022). https://doi.org/10.1557/s43577-021-00195-0

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