Rebecca Lalk , Yauhen Tratsiak , Nicholas Anastasi , Luis Stand , Charles L. Melcher , Mariya Zhuravleva
{"title":"组成络合物(Gd1/4Y1/4Tb1/4Lu1/4)3Al5O12:Ce单晶闪烁体中的能量迁移和闪烁动力学","authors":"Rebecca Lalk , Yauhen Tratsiak , Nicholas Anastasi , Luis Stand , Charles L. Melcher , Mariya Zhuravleva","doi":"10.1016/j.jlumin.2025.121494","DOIUrl":null,"url":null,"abstract":"<div><div>It is well-established that compositional tuning through binary admixture can improve scintillation performance in several materials systems, including Ce-activated garnets. Although recent work on ternary or quaternary cation admixture shows promise, the impact of this increased compositional complexity on thermal stability and carrier-defect dynamics has not been addressed. Here, we investigate a compositionally complex garnet, (Gd<sub>1/4</sub>Y<sub>1/4</sub>Tb<sub>1/4</sub>Lu<sub>1/4</sub>)<sub>3</sub>Al<sub>5</sub>O<sub>12</sub>:Ce (GYTLAG), grown by the Czochralski method using temperature-dependent photoluminescence (PL), PL decay, and thermoluminescence (TL). PL and PL decay measurements support a thermally activated Tb<sup>3+</sup>-Ce<sup>3+</sup> energy transfer, where Tb<sup>3+</sup> emission dominates below 60 K, but Ce<sup>3+</sup> emission increases from 20 to 300 K. Thermal quenching of Ce<sup>3+</sup> emission occurs around <em>T</em><sub><em>50</em></sub> = 508 K, with an activation energy of 0.6 eV. TL and wavelength-resolved TL spectra from 20 to 500 K show that GYTLAG contains similar trap groups to LuAG but with a broader distribution of glow peaks below room temperature, possibly caused by quaternary cation mixing. A combination of dose dependence, partial cleaning and initial rise, and glow curve fitting to a first order continuous Gaussian distribution model are used to understand the contribution of electronic point defects to scintillation decay and afterglow at room temperature. These results inform how increased compositional complexity influences recombination dynamics in garnet scintillators.</div></div>","PeriodicalId":16159,"journal":{"name":"Journal of Luminescence","volume":"287 ","pages":"Article 121494"},"PeriodicalIF":3.6000,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Energy migration and scintillation kinetics in compositionally complex (Gd1/4Y1/4Tb1/4Lu1/4)3Al5O12:Ce single crystal scintillator\",\"authors\":\"Rebecca Lalk , Yauhen Tratsiak , Nicholas Anastasi , Luis Stand , Charles L. Melcher , Mariya Zhuravleva\",\"doi\":\"10.1016/j.jlumin.2025.121494\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>It is well-established that compositional tuning through binary admixture can improve scintillation performance in several materials systems, including Ce-activated garnets. Although recent work on ternary or quaternary cation admixture shows promise, the impact of this increased compositional complexity on thermal stability and carrier-defect dynamics has not been addressed. Here, we investigate a compositionally complex garnet, (Gd<sub>1/4</sub>Y<sub>1/4</sub>Tb<sub>1/4</sub>Lu<sub>1/4</sub>)<sub>3</sub>Al<sub>5</sub>O<sub>12</sub>:Ce (GYTLAG), grown by the Czochralski method using temperature-dependent photoluminescence (PL), PL decay, and thermoluminescence (TL). PL and PL decay measurements support a thermally activated Tb<sup>3+</sup>-Ce<sup>3+</sup> energy transfer, where Tb<sup>3+</sup> emission dominates below 60 K, but Ce<sup>3+</sup> emission increases from 20 to 300 K. Thermal quenching of Ce<sup>3+</sup> emission occurs around <em>T</em><sub><em>50</em></sub> = 508 K, with an activation energy of 0.6 eV. TL and wavelength-resolved TL spectra from 20 to 500 K show that GYTLAG contains similar trap groups to LuAG but with a broader distribution of glow peaks below room temperature, possibly caused by quaternary cation mixing. A combination of dose dependence, partial cleaning and initial rise, and glow curve fitting to a first order continuous Gaussian distribution model are used to understand the contribution of electronic point defects to scintillation decay and afterglow at room temperature. These results inform how increased compositional complexity influences recombination dynamics in garnet scintillators.</div></div>\",\"PeriodicalId\":16159,\"journal\":{\"name\":\"Journal of Luminescence\",\"volume\":\"287 \",\"pages\":\"Article 121494\"},\"PeriodicalIF\":3.6000,\"publicationDate\":\"2025-08-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Luminescence\",\"FirstCategoryId\":\"101\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S002223132500434X\",\"RegionNum\":3,\"RegionCategory\":\"物理与天体物理\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"OPTICS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Luminescence","FirstCategoryId":"101","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S002223132500434X","RegionNum":3,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"OPTICS","Score":null,"Total":0}
Energy migration and scintillation kinetics in compositionally complex (Gd1/4Y1/4Tb1/4Lu1/4)3Al5O12:Ce single crystal scintillator
It is well-established that compositional tuning through binary admixture can improve scintillation performance in several materials systems, including Ce-activated garnets. Although recent work on ternary or quaternary cation admixture shows promise, the impact of this increased compositional complexity on thermal stability and carrier-defect dynamics has not been addressed. Here, we investigate a compositionally complex garnet, (Gd1/4Y1/4Tb1/4Lu1/4)3Al5O12:Ce (GYTLAG), grown by the Czochralski method using temperature-dependent photoluminescence (PL), PL decay, and thermoluminescence (TL). PL and PL decay measurements support a thermally activated Tb3+-Ce3+ energy transfer, where Tb3+ emission dominates below 60 K, but Ce3+ emission increases from 20 to 300 K. Thermal quenching of Ce3+ emission occurs around T50 = 508 K, with an activation energy of 0.6 eV. TL and wavelength-resolved TL spectra from 20 to 500 K show that GYTLAG contains similar trap groups to LuAG but with a broader distribution of glow peaks below room temperature, possibly caused by quaternary cation mixing. A combination of dose dependence, partial cleaning and initial rise, and glow curve fitting to a first order continuous Gaussian distribution model are used to understand the contribution of electronic point defects to scintillation decay and afterglow at room temperature. These results inform how increased compositional complexity influences recombination dynamics in garnet scintillators.
期刊介绍:
The purpose of the Journal of Luminescence is to provide a means of communication between scientists in different disciplines who share a common interest in the electronic excited states of molecular, ionic and covalent systems, whether crystalline, amorphous, or liquid.
We invite original papers and reviews on such subjects as: exciton and polariton dynamics, dynamics of localized excited states, energy and charge transport in ordered and disordered systems, radiative and non-radiative recombination, relaxation processes, vibronic interactions in electronic excited states, photochemistry in condensed systems, excited state resonance, double resonance, spin dynamics, selective excitation spectroscopy, hole burning, coherent processes in excited states, (e.g. coherent optical transients, photon echoes, transient gratings), multiphoton processes, optical bistability, photochromism, and new techniques for the study of excited states. This list is not intended to be exhaustive. Papers in the traditional areas of optical spectroscopy (absorption, MCD, luminescence, Raman scattering) are welcome. Papers on applications (phosphors, scintillators, electro- and cathodo-luminescence, radiography, bioimaging, solar energy, energy conversion, etc.) are also welcome if they present results of scientific, rather than only technological interest. However, papers containing purely theoretical results, not related to phenomena in the excited states, as well as papers using luminescence spectroscopy to perform routine analytical chemistry or biochemistry procedures, are outside the scope of the journal. Some exceptions will be possible at the discretion of the editors.