{"title":"Quantitatively Deciphering the Local Structure and Luminescence Spectroscopy of Pr<sup>3+</sup>-Doped Yttrium Lithium Fluoride.","authors":"Yang Xiao, Qiang Luo, Meng Ju, Yauyuen Yeung","doi":"10.1021/acs.jpca.4c03698","DOIUrl":null,"url":null,"abstract":"<p><p>Praseodymium (Pr<sup>3+</sup>)-doped LiYF<sub>4</sub> nanophosphors have garnered significant interest for their potential applications in lasers, phosphors, and quantum memories. However, there remains a lack of comprehensive research on the local coordination environment and luminescence spectroscopy of Pr<sup>3+</sup>:LiYF<sub>4</sub> nanocrystals. This study presents the first investigation of the ground-state structure of Pr<sup>3+</sup>:LiYF<sub>4</sub> crystals by employing the crystal structure prediction method, and a [PrF<sub>8</sub>]<sup>5-</sup> ligand complex with <i>S</i><sub><i>4</i></sub> local symmetry is determined. The complete energy levels of the Pr<sup>3+</sup> ions in LiYF<sub>4</sub> nanocrystals are unveiled by using our newly developed well-established parametrization matrix diagonalization method. A novel set of free-ion and crystal-field parameters is derived through a good simulation with 45 experimental energy levels. Many of the emissions of Pr<sup>3+</sup>-doped LiYF<sub>4</sub> are successfully reproduced based on Judd-Ofelt theory, and these transitions are comparable to the experimental ones. Moreover, two new prominent emission bands with their peaks at 675 and 849 nm originating from <sup>1</sup>I<sub>6</sub> → <sup>3</sup>F<sub>4</sub> and <sup>1</sup>I<sub>6</sub> → <sup>1</sup>G<sub>4</sub> transitions, respectively, are predicted by us for the first time. This study could provide a feasible method to search for practical laser transition channels of solid-state lasers based on Pr<sup>3+</sup>: LiYF<sub>4</sub> nanophosphors.</p>","PeriodicalId":59,"journal":{"name":"The Journal of Physical Chemistry A","volume":null,"pages":null},"PeriodicalIF":2.7000,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry A","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.jpca.4c03698","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Praseodymium (Pr3+)-doped LiYF4 nanophosphors have garnered significant interest for their potential applications in lasers, phosphors, and quantum memories. However, there remains a lack of comprehensive research on the local coordination environment and luminescence spectroscopy of Pr3+:LiYF4 nanocrystals. This study presents the first investigation of the ground-state structure of Pr3+:LiYF4 crystals by employing the crystal structure prediction method, and a [PrF8]5- ligand complex with S4 local symmetry is determined. The complete energy levels of the Pr3+ ions in LiYF4 nanocrystals are unveiled by using our newly developed well-established parametrization matrix diagonalization method. A novel set of free-ion and crystal-field parameters is derived through a good simulation with 45 experimental energy levels. Many of the emissions of Pr3+-doped LiYF4 are successfully reproduced based on Judd-Ofelt theory, and these transitions are comparable to the experimental ones. Moreover, two new prominent emission bands with their peaks at 675 and 849 nm originating from 1I6 → 3F4 and 1I6 → 1G4 transitions, respectively, are predicted by us for the first time. This study could provide a feasible method to search for practical laser transition channels of solid-state lasers based on Pr3+: LiYF4 nanophosphors.
期刊介绍:
The Journal of Physical Chemistry A is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.