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LuAlScGaO晶体中结构无序与Pr发射动力学的关联:全面的结构-性质研究

Correlating Structural Disorder and Pr Emission Dynamics in LuAl Sc GaO Crystals: A Comprehensive Structure-Property Investigation.

作者信息

Bartosiewicz Karol, Dewo Wioletta, Nagirnyi Vitali, Runka Tomasz, Kirm Marco, Horiai Takahiko, Szymanski Damian, Yamaji Akihiro, Kurosawa Shunsuke, Socha Paweł, Pejchal Jan, Babin Vladimir, Kral Robert, Kotlov Aleksei, Yoshikawa Akira, Nikl Martin

机构信息

Institute of Physics, Academy of Sciences of the Czech Republic, Na Slovance 1999/2, Praha 18200, Czechia.

Faculty of Materials Engineering and Technical Physics, Poznan University of Technology, Piotrowo 3, Poznań 60965, Poland.

出版信息

ACS Omega. 2025 May 8;10(19):19817-19831. doi: 10.1021/acsomega.5c01062. eCollection 2025 May 20.

Abstract

This study explored the influence of Sc ions incorporation on the structural, vibrational, luminescent, and scintillation properties of Pr-doped Lu(Al, Sc)GaO garnet crystals. Addressing the limited research on Sc-admixed and Pr doped garnet systems, this work successfully demonstrated the crystallization of garnet crystals from the melt, overcoming the substantial atomic mismatch between Sc and Al while preserving the thermodynamic stability of the garnet phase. Importantly, Sc-admixing enhanced atomic homogeneity and allowed for increased doping concentrations of Pr ions, which is crucial for tailoring the functional properties of advanced optical materials. The trap depths ranged from 1.63 eV (deep traps) to 0.22 eV (shallow traps) across all samples, with frequency factors predominantly between 1 × 10 and 1 × 10 s, consistent with first-order thermoluminescent kinetics. From a materials design perspective, Sc ions substitution induced beneficial host lattice disorder, enhancing the emission intensity of 4f5d → 4f interconfigurational and 4f → 4f intraconfigurational transitions. This effect highlighted the potential of Sc as a promising substituent for enhancing the luminescence intensity of rare earth elements. Synchrotron radiation experiments provided insights into the impact of Sc on band gap energy and energy transfer efficiency toward Pr ions offering new opportunities for engineering scintillators and phosphors with tunable optical properties.

摘要

本研究探讨了掺入Sc离子对掺Pr的Lu(Al, Sc)GaO石榴石晶体的结构、振动、发光和闪烁性能的影响。针对Sc掺杂和Pr掺杂石榴石体系研究有限的情况,本工作成功证明了石榴石晶体从熔体中结晶,克服了Sc与Al之间的巨大原子失配,同时保持了石榴石相的热力学稳定性。重要的是,Sc掺杂提高了原子均匀性,并允许提高Pr离子的掺杂浓度,这对于定制先进光学材料的功能特性至关重要。所有样品的陷阱深度范围为1.63 eV(深陷阱)至0.22 eV(浅陷阱),频率因子主要在1×10至1×10 s之间,符合一级热释光动力学。从材料设计的角度来看,Sc离子取代引起了有益的基质晶格无序,增强了4f5d→4f组态间跃迁和4f→4f组态内跃迁的发射强度。这种效应突出了Sc作为增强稀土元素发光强度的有前景替代物的潜力。同步辐射实验提供了关于Sc对带隙能量的影响以及向Pr离子的能量转移效率的见解,为设计具有可调光学性能的闪烁体和磷光体提供了新机会。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f7d2/12096190/4a153245ed1c/ao5c01062_0001.jpg

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