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Lanthanides (Ln3+) doped luminescent materials play critical roles in lighting and display techniques. While increasing experimental and theoretical research have been carried out on aluminate-based phosphors for white light-emitting diodes (WLEDs) over the past decades, most investigation was mainly focused on their luminescent properties; therefore, the local structure of the light emission center remains unclear. Especially, doping-induced local composition and structure modification around the luminescent centers have yet to be unveiled. In this study, we use advanced electron microscopy techniques including electron diffraction (ED), high-resolution transmission electron microscopy (HRTEM), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), in combination with energy dispersive X-ray spectroscopy (EDX) and electron energy loss spectroscopy (EELS), to reveal atomically resolved crystalline and chemical structure of Ce3+ doped CaYAlO4. The microscopic results prove substantial microstructural and compositional inhomogeneities in Ce3+ doped CaYAlO4, especially the appearance of Ce dopant clustering and Ce3+/Ce4+ valence variation. Our research provides a new understanding the structure of Ln3+ doped luminescent materials and will facilitate the materials design for next-generation WLEDs luminescent materials.

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Publication history

Received: 07 June 2022
Revised: 19 July 2022
Accepted: 07 August 2022
Published: 21 September 2022

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© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was funded by the National Natural Science Foundation of China (Nos. 52002357, 22105175, and 51932009). P. L. acknowledges the financial support from the Carlsberg Foundation (No. CF20-0612). We acknowledge Dr. Zhao for providing the sample and Center of Advanced Analysis & Gene Sequencing, Zhengzhou University for the advanced electron microscopy facilities.

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Email: nanores@tup.tsinghua.edu.cn

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