{"title":"Cs2NaGdCl6:Tb3+--用于低剂量 X 射线探测和成像的高发光稀土双包晶闪烁体","authors":"Varnakavi Naresh, Pil-Ryung Cha* and Nohyun Lee*, ","doi":"10.1021/acsami.3c17301","DOIUrl":null,"url":null,"abstract":"<p >Rare-earth-based double perovskite (DP) X-ray scintillators have gained significant importance with low detection limits in medical imaging and radiation detection owing to their high light yield (LY) and remarkable spatial resolution. Herein, we report the synthesis of 3D double perovskite (DP) crystals, namely, Cs<sub>2</sub>NaGdCl<sub>6</sub> and Tb<sup>3+</sup>-Cs<sub>2</sub>NaGdCl<sub>6</sub> using hydrothermal reaction. Cs<sub>2</sub>NaGdCl<sub>6</sub> DP single crystals exhibited a blue self-trapped exciton (STE) emission at 470 nm under ultraviolet (265 nm) excitation with a photoluminescence quantum yield (PLQY) of 8.4%. Introducing Tb<sup>3+</sup> ions into Cs<sub>2</sub>NaGdCl<sub>6</sub> has resulted in quenching of STE emission and enhancing green emission at 549 nm attributed to the <sup>5</sup>D<sub>4</sub> → <sup>7</sup>F<sub>5</sub> transition of Tb<sup>3+</sup>, suggesting efficient energy transfer (ET) from STE to Tb<sup>3+</sup>. This ET process is evidenced by the appearance of Tb<sup>3+</sup> bands in the excitation spectra of the host, the shortening of the STE lifetimes in the presence of Tb<sup>3+</sup> ions, and the enhancement of PLQY (72.6%). Furthermore, Cs<sub>2</sub>NaGdCl<sub>6</sub>:5%Tb<sup>3+</sup> films of various thicknesses (0.1–0.6 mm) were synthesized and their X-ray scintillating performance has been examined. The Cs<sub>2</sub>NaGdCl<sub>6</sub>:5%Tb<sup>3+</sup> film with 0.4 mm thickness has exhibited an excellent linear response to the X-ray dose rate with a low detection limit of 41.32 nGy<sub>air</sub> s<sup>–1</sup>, an LY of 39,100 photons MeV<sup>–1</sup>, and excellent radiation stability. Benefiting from the strong X-ray excited luminescence (XEL) of Cs<sub>2</sub>NaGdCl<sub>6</sub>:5%Tb<sup>3+</sup>, we developed a Cs<sub>2</sub>NaGdCl<sub>6</sub>:5%Tb<sup>3+</sup> X-ray scintillator screen with a least thickness (0.1 mm), exhibiting remarkable imaging ability with a spatial resolution of 10.75 lp mm<sup>–1</sup>. These results suggest that Cs<sub>2</sub>NaGdCl<sub>6</sub>:Tb<sup>3+</sup> can be a potential candidate for low-dose and X-ray imaging applications.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"16 15","pages":"19068–19080"},"PeriodicalIF":8.3000,"publicationDate":"2024-04-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Cs2NaGdCl6:Tb3+─A Highly Luminescent Rare-Earth Double Perovskite Scintillator for Low-Dose X-ray Detection and Imaging\",\"authors\":\"Varnakavi Naresh, Pil-Ryung Cha* and Nohyun Lee*, \",\"doi\":\"10.1021/acsami.3c17301\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Rare-earth-based double perovskite (DP) X-ray scintillators have gained significant importance with low detection limits in medical imaging and radiation detection owing to their high light yield (LY) and remarkable spatial resolution. Herein, we report the synthesis of 3D double perovskite (DP) crystals, namely, Cs<sub>2</sub>NaGdCl<sub>6</sub> and Tb<sup>3+</sup>-Cs<sub>2</sub>NaGdCl<sub>6</sub> using hydrothermal reaction. Cs<sub>2</sub>NaGdCl<sub>6</sub> DP single crystals exhibited a blue self-trapped exciton (STE) emission at 470 nm under ultraviolet (265 nm) excitation with a photoluminescence quantum yield (PLQY) of 8.4%. Introducing Tb<sup>3+</sup> ions into Cs<sub>2</sub>NaGdCl<sub>6</sub> has resulted in quenching of STE emission and enhancing green emission at 549 nm attributed to the <sup>5</sup>D<sub>4</sub> → <sup>7</sup>F<sub>5</sub> transition of Tb<sup>3+</sup>, suggesting efficient energy transfer (ET) from STE to Tb<sup>3+</sup>. This ET process is evidenced by the appearance of Tb<sup>3+</sup> bands in the excitation spectra of the host, the shortening of the STE lifetimes in the presence of Tb<sup>3+</sup> ions, and the enhancement of PLQY (72.6%). Furthermore, Cs<sub>2</sub>NaGdCl<sub>6</sub>:5%Tb<sup>3+</sup> films of various thicknesses (0.1–0.6 mm) were synthesized and their X-ray scintillating performance has been examined. The Cs<sub>2</sub>NaGdCl<sub>6</sub>:5%Tb<sup>3+</sup> film with 0.4 mm thickness has exhibited an excellent linear response to the X-ray dose rate with a low detection limit of 41.32 nGy<sub>air</sub> s<sup>–1</sup>, an LY of 39,100 photons MeV<sup>–1</sup>, and excellent radiation stability. Benefiting from the strong X-ray excited luminescence (XEL) of Cs<sub>2</sub>NaGdCl<sub>6</sub>:5%Tb<sup>3+</sup>, we developed a Cs<sub>2</sub>NaGdCl<sub>6</sub>:5%Tb<sup>3+</sup> X-ray scintillator screen with a least thickness (0.1 mm), exhibiting remarkable imaging ability with a spatial resolution of 10.75 lp mm<sup>–1</sup>. These results suggest that Cs<sub>2</sub>NaGdCl<sub>6</sub>:Tb<sup>3+</sup> can be a potential candidate for low-dose and X-ray imaging applications.</p>\",\"PeriodicalId\":5,\"journal\":{\"name\":\"ACS Applied Materials & Interfaces\",\"volume\":\"16 15\",\"pages\":\"19068–19080\"},\"PeriodicalIF\":8.3000,\"publicationDate\":\"2024-04-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Materials & Interfaces\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acsami.3c17301\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Materials & Interfaces","FirstCategoryId":"88","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsami.3c17301","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
Cs2NaGdCl6:Tb3+─A Highly Luminescent Rare-Earth Double Perovskite Scintillator for Low-Dose X-ray Detection and Imaging
Rare-earth-based double perovskite (DP) X-ray scintillators have gained significant importance with low detection limits in medical imaging and radiation detection owing to their high light yield (LY) and remarkable spatial resolution. Herein, we report the synthesis of 3D double perovskite (DP) crystals, namely, Cs2NaGdCl6 and Tb3+-Cs2NaGdCl6 using hydrothermal reaction. Cs2NaGdCl6 DP single crystals exhibited a blue self-trapped exciton (STE) emission at 470 nm under ultraviolet (265 nm) excitation with a photoluminescence quantum yield (PLQY) of 8.4%. Introducing Tb3+ ions into Cs2NaGdCl6 has resulted in quenching of STE emission and enhancing green emission at 549 nm attributed to the 5D4 → 7F5 transition of Tb3+, suggesting efficient energy transfer (ET) from STE to Tb3+. This ET process is evidenced by the appearance of Tb3+ bands in the excitation spectra of the host, the shortening of the STE lifetimes in the presence of Tb3+ ions, and the enhancement of PLQY (72.6%). Furthermore, Cs2NaGdCl6:5%Tb3+ films of various thicknesses (0.1–0.6 mm) were synthesized and their X-ray scintillating performance has been examined. The Cs2NaGdCl6:5%Tb3+ film with 0.4 mm thickness has exhibited an excellent linear response to the X-ray dose rate with a low detection limit of 41.32 nGyair s–1, an LY of 39,100 photons MeV–1, and excellent radiation stability. Benefiting from the strong X-ray excited luminescence (XEL) of Cs2NaGdCl6:5%Tb3+, we developed a Cs2NaGdCl6:5%Tb3+ X-ray scintillator screen with a least thickness (0.1 mm), exhibiting remarkable imaging ability with a spatial resolution of 10.75 lp mm–1. These results suggest that Cs2NaGdCl6:Tb3+ can be a potential candidate for low-dose and X-ray imaging applications.
期刊介绍:
ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.