Dagmara Kulesza, Justyna Zeler, Markus Suta, Eugeniusz Zych
{"title":"从深低温到极热:解锁Pr3+活化Ca3Sc2Si3O12和Ca3Sc2Ge3O12石榴石的单离子发光测温","authors":"Dagmara Kulesza, Justyna Zeler, Markus Suta, Eugeniusz Zych","doi":"10.1021/acs.chemmater.5c01216","DOIUrl":null,"url":null,"abstract":"Luminescence thermometry is gaining prominence as a noncontact-reading temperature sensing technique, offering high precision, robustness, and material tunability. In this work, we report Pr<sup>3+</sup>-doped garnets, Ca<sub>3</sub>Sc<sub>2</sub>Si<sub>3</sub>O<sub>12</sub>:0.1% Pr and Ca<sub>3</sub>Sc<sub>2</sub>Ge<sub>3</sub>O<sub>12</sub>:0.1% Pr, as promising candidates for wide-range optical thermometry based on both emission intensity and decay time metrics. The silicate garnet exhibits a record operational range of 25–1225 K, with relative thermal sensitivity spanning 0.5–1.3%·K<sup>–1</sup> over 250–1225 K, sustained by intense and thermally controlled 4f<sup>1</sup>5d<sup>1</sup> → 4f<sup>2</sup> emission. Temperature-dependent luminescence measurements reveal a continuous and monotonic decrease in both emission intensity and lifetime, supporting two-modal reliable, quantitative thermal readout. At elevated temperatures (≥900 K), thermally stimulated back-transfer from the <sup>1</sup>D<sub>2</sub> to the <sup>3</sup>P<sub>0</sub> level activates an additional <sup>3</sup>P<sub>0</sub>/<sup>1</sup>D<sub>2</sub> intensity ratio metric, achieving 0.44%·K<sup>–1</sup> sensitivity. The germanate counterpart shows strong performance in the 20–225 K range, with relative sensitivities exceeding 5%·K<sup>–1</sup>. These Pr<sup>3+</sup>-activated phosphors, featuring submicron particle size, phase stability, and broad thermal response, enable multimodal, single-ion thermometry across a continuous, ultrawide temperature span. These findings highlight the potential of garnet hosts for next-generation luminescent thermometers in high-demand environments such as catalysis, aerospace, nuclear monitoring, and space exploration.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"1 1","pages":""},"PeriodicalIF":7.0000,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"From Deep Cryogenics to Extreme Heat: Unlocking Single-Ion Luminescent Thermometry with Pr3+-Activated Ca3Sc2Si3O12 and Ca3Sc2Ge3O12 Garnets\",\"authors\":\"Dagmara Kulesza, Justyna Zeler, Markus Suta, Eugeniusz Zych\",\"doi\":\"10.1021/acs.chemmater.5c01216\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Luminescence thermometry is gaining prominence as a noncontact-reading temperature sensing technique, offering high precision, robustness, and material tunability. In this work, we report Pr<sup>3+</sup>-doped garnets, Ca<sub>3</sub>Sc<sub>2</sub>Si<sub>3</sub>O<sub>12</sub>:0.1% Pr and Ca<sub>3</sub>Sc<sub>2</sub>Ge<sub>3</sub>O<sub>12</sub>:0.1% Pr, as promising candidates for wide-range optical thermometry based on both emission intensity and decay time metrics. The silicate garnet exhibits a record operational range of 25–1225 K, with relative thermal sensitivity spanning 0.5–1.3%·K<sup>–1</sup> over 250–1225 K, sustained by intense and thermally controlled 4f<sup>1</sup>5d<sup>1</sup> → 4f<sup>2</sup> emission. Temperature-dependent luminescence measurements reveal a continuous and monotonic decrease in both emission intensity and lifetime, supporting two-modal reliable, quantitative thermal readout. At elevated temperatures (≥900 K), thermally stimulated back-transfer from the <sup>1</sup>D<sub>2</sub> to the <sup>3</sup>P<sub>0</sub> level activates an additional <sup>3</sup>P<sub>0</sub>/<sup>1</sup>D<sub>2</sub> intensity ratio metric, achieving 0.44%·K<sup>–1</sup> sensitivity. The germanate counterpart shows strong performance in the 20–225 K range, with relative sensitivities exceeding 5%·K<sup>–1</sup>. These Pr<sup>3+</sup>-activated phosphors, featuring submicron particle size, phase stability, and broad thermal response, enable multimodal, single-ion thermometry across a continuous, ultrawide temperature span. These findings highlight the potential of garnet hosts for next-generation luminescent thermometers in high-demand environments such as catalysis, aerospace, nuclear monitoring, and space exploration.\",\"PeriodicalId\":33,\"journal\":{\"name\":\"Chemistry of Materials\",\"volume\":\"1 1\",\"pages\":\"\"},\"PeriodicalIF\":7.0000,\"publicationDate\":\"2025-09-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemistry of Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.chemmater.5c01216\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemistry of Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acs.chemmater.5c01216","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
From Deep Cryogenics to Extreme Heat: Unlocking Single-Ion Luminescent Thermometry with Pr3+-Activated Ca3Sc2Si3O12 and Ca3Sc2Ge3O12 Garnets
Luminescence thermometry is gaining prominence as a noncontact-reading temperature sensing technique, offering high precision, robustness, and material tunability. In this work, we report Pr3+-doped garnets, Ca3Sc2Si3O12:0.1% Pr and Ca3Sc2Ge3O12:0.1% Pr, as promising candidates for wide-range optical thermometry based on both emission intensity and decay time metrics. The silicate garnet exhibits a record operational range of 25–1225 K, with relative thermal sensitivity spanning 0.5–1.3%·K–1 over 250–1225 K, sustained by intense and thermally controlled 4f15d1 → 4f2 emission. Temperature-dependent luminescence measurements reveal a continuous and monotonic decrease in both emission intensity and lifetime, supporting two-modal reliable, quantitative thermal readout. At elevated temperatures (≥900 K), thermally stimulated back-transfer from the 1D2 to the 3P0 level activates an additional 3P0/1D2 intensity ratio metric, achieving 0.44%·K–1 sensitivity. The germanate counterpart shows strong performance in the 20–225 K range, with relative sensitivities exceeding 5%·K–1. These Pr3+-activated phosphors, featuring submicron particle size, phase stability, and broad thermal response, enable multimodal, single-ion thermometry across a continuous, ultrawide temperature span. These findings highlight the potential of garnet hosts for next-generation luminescent thermometers in high-demand environments such as catalysis, aerospace, nuclear monitoring, and space exploration.
期刊介绍:
The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.