Theoretical determination of the electronic structures and energy-level splitting for Pr³⁺-doped YSiO crystals

Wenhao JI, Meng JU, Hongkuan YUAN, Yang XIAO, Yau Yuen YEUNG

Research output: Contribution to journalArticlespeer-review

Abstract

Trivalent praseodymium (Pr³⁺)-doped yttrium silicate (YSiO) crystals have been widely used in various phosphors owing to their excellent luminescence characteristics. Although a series of studies have been carried out on its application prospects, the electronic structures and energy-transfer mechanisms of Pr³⁺-doped YSiO (YSiO:Pr) remain an exploratory topic. Herein, the crystal structure analysis by the particle swarm optimization structure search method is used to study the structural evolution of YSiO:Pr. Two novel structures with local [PrO7]⁻¹¹ and [PrO]⁻⁹ [YSiO:Pr (I) and YSiO:Pr (II)] are successfully identified. The impurity Pr³⁺ ions occupy the Y³⁺ sites and successfully integrate into the YSiO host crystal with a Pr³⁺ concentration of 6.25%. The calculated electronic band structures show that the doping of Pr³⁺ induces a reduction in band gaps for the host YSiO crystal. The conduction bands near the Fermi level are completely composed of f states. For the atomic energies of Pr³⁺ in YSiO, the Stark levels and transitions are properly simulated based on a new set of crystal field parameters (CFPs) at the C site symmetry. A satisfactory r.m.s. dev. of 15.57 cm⁻¹ with 9 free ion parameters (plus 27 fixed CFPs as obtained from ab initio calculation) fitted to the 33 observed levels is obtained for the first time. The plentiful energy-level transition lines, from the visible light to the near-infrared region, are deciphered for Pr³⁺ in YSiO. Blue ³P0 → ³H at 465 nm is calculated to be a strong emission line, and it might be an ideal channel for laser actions. These results could not only provide important insights into the rare-earth-doped crystals but also lay the foundation for future research studies of designing the new laser materials. Copyright © 2024 American Chemical Society.

Original languageEnglish
JournalJournal of Physical Chemistry A
Early online dateMay 2024
DOIs
Publication statusE-pub ahead of print - May 2024

Citation

Ji, W., Ju, M., Yuan, H., Xiao, Y., & Yeung, Y.-Y. (2024). Theoretical determination of the electronic structures and energy-level splitting for Pr³⁺-doped Y₂SiO₅ crystals. Journal of Physical Chemistry A. Advance online publication. https://doi.org/10.1021/acs.jpca.4c01251

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