{"title":"Removal of deep traps in Lu2O3:Tm phosphors via formation of continuous solid solutions with In2O3 enabling widely tailorable bandgap energy","authors":"","doi":"10.1016/j.apt.2024.104610","DOIUrl":null,"url":null,"abstract":"<div><p>Bandgap engineering has been effectively used to reduce the shallow-trap defects (<em>e</em>.<em>g</em>. antisite defects), but there are still rare reports on the removal of deep-trap defects (<em>e</em>.<em>g</em>. oxygen defects). In this work, our proposed strategy of In<sup>3+</sup> substitution for Lu<sup>3+</sup> via the formation of continuous (Lu,In)<sub>2</sub>O<sub>3</sub> solid solutions can be used to widely tailored the bandgap energy. These solid solutions prepared from the chemical co-precipitation route presented the rounded morphology and their particle sizes increased at a higher In<sup>3+</sup> content. The (Lu,In)<sub>2</sub>O<sub>3</sub>:Tm phosphor powders exhibited characteristic Tm<sup>3+</sup> emissions arising from its intra‐4<em>f</em><sup>12</sup> multi‐transitions upon UV excitation into strong broad charge transfer bands. The luminescence intensity reached the highest level at 15 at.% In<sup>3+</sup> concentration. The In<sup>3+</sup> incorporation was found to red-shift the charge transfer bands and shortened the florescence lifetimes. The luminescence quenching was dominated by exchange interaction while the theoretical and experimental quenching concentration of Tm<sup>3+</sup> coincided well with each other (both ∼1 at.%). The trap depth in the In<sup>3+</sup> free Lu<sub>2</sub>O<sub>3</sub>:Tm phosphor was determined to be ∼0.61 eV and these electron traps could be almost fully buried at the In<sup>3+</sup> concentration above 5 at.%. Both the (Lu<sub>0.99</sub>Tm<sub>0.01</sub>)<sub>2</sub>O<sub>3</sub> and (Lu<sub>0.84</sub>In<sub>0.15</sub>Tm<sub>0.01</sub>)<sub>2</sub>O<sub>3</sub> phosphors exhibited good thermal stability with high thermal-quenching activation energies (∼0.45 eV for the former and ∼0.39 eV for the latter). However, the (Lu<sub>0.99</sub>Tm<sub>0.01</sub>)<sub>2</sub>O<sub>3</sub> phosphor presented abnormal thermal quenching effect.</p></div>","PeriodicalId":7232,"journal":{"name":"Advanced Powder Technology","volume":null,"pages":null},"PeriodicalIF":4.2000,"publicationDate":"2024-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Powder Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0921883124002863","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Bandgap engineering has been effectively used to reduce the shallow-trap defects (e.g. antisite defects), but there are still rare reports on the removal of deep-trap defects (e.g. oxygen defects). In this work, our proposed strategy of In3+ substitution for Lu3+ via the formation of continuous (Lu,In)2O3 solid solutions can be used to widely tailored the bandgap energy. These solid solutions prepared from the chemical co-precipitation route presented the rounded morphology and their particle sizes increased at a higher In3+ content. The (Lu,In)2O3:Tm phosphor powders exhibited characteristic Tm3+ emissions arising from its intra‐4f12 multi‐transitions upon UV excitation into strong broad charge transfer bands. The luminescence intensity reached the highest level at 15 at.% In3+ concentration. The In3+ incorporation was found to red-shift the charge transfer bands and shortened the florescence lifetimes. The luminescence quenching was dominated by exchange interaction while the theoretical and experimental quenching concentration of Tm3+ coincided well with each other (both ∼1 at.%). The trap depth in the In3+ free Lu2O3:Tm phosphor was determined to be ∼0.61 eV and these electron traps could be almost fully buried at the In3+ concentration above 5 at.%. Both the (Lu0.99Tm0.01)2O3 and (Lu0.84In0.15Tm0.01)2O3 phosphors exhibited good thermal stability with high thermal-quenching activation energies (∼0.45 eV for the former and ∼0.39 eV for the latter). However, the (Lu0.99Tm0.01)2O3 phosphor presented abnormal thermal quenching effect.
带隙工程已被有效地用于减少浅阱缺陷(.反位错缺陷),但关于消除深阱缺陷(.氧缺陷)的报道仍然很少。在这项工作中,我们提出了通过形成连续的(Lu,In)O 固溶体用 In 替代 Lu 的策略,可用于广泛调整带隙能。这些通过化学共沉淀路线制备的固溶体呈现出圆形的形态,并且当 In 含量越高时,其粒径也越大。(Lu,In)O:Tm荧光粉在紫外光激发下会发生4内多跃迁,形成强宽的电荷转移带,从而产生特征性的Tm发射。当 In 浓度为 15%时,发光强度达到最高水平。铟的掺入使电荷转移带发生红移,并缩短了荧光寿命。发光淬灭主要是由交换相互作用引起的,而 Tm 的理论淬灭浓度和实验淬灭浓度非常吻合(均为 1 at.%)。无 In 的 LuO:Tm 荧光粉中的陷阱深度被测定为 ∼0.61 eV,当 In 浓度超过 5 at.% 时,这些电子陷阱几乎可以完全埋藏。(LuTm)O和(LuInTm)O荧光粉都具有良好的热稳定性,热淬灭活化能较高(前者为0.45 eV,后者为0.39 eV)。然而,(LuTm)O 荧光粉却表现出异常的热淬火效应。
期刊介绍:
The aim of Advanced Powder Technology is to meet the demand for an international journal that integrates all aspects of science and technology research on powder and particulate materials. The journal fulfills this purpose by publishing original research papers, rapid communications, reviews, and translated articles by prominent researchers worldwide.
The editorial work of Advanced Powder Technology, which was founded as the International Journal of the Society of Powder Technology, Japan, is now shared by distinguished board members, who operate in a unique framework designed to respond to the increasing global demand for articles on not only powder and particles, but also on various materials produced from them.
Advanced Powder Technology covers various areas, but a discussion of powder and particles is required in articles. Topics include: Production of powder and particulate materials in gases and liquids(nanoparticles, fine ceramics, pharmaceuticals, novel functional materials, etc.); Aerosol and colloidal processing; Powder and particle characterization; Dynamics and phenomena; Calculation and simulation (CFD, DEM, Monte Carlo method, population balance, etc.); Measurement and control of powder processes; Particle modification; Comminution; Powder handling and operations (storage, transport, granulation, separation, fluidization, etc.)