Abnormal dielectric behavior of glaserite-type Ba3−xSrxMgSi2O8 solid solution

The temperature coefficient of the resonant frequency (τf) of low-permittivity (εr) microwave dielectric ceramics is required to be near 0 ppm/°C for practical application. However, owing to the polarization mechanism, τf of low-εr microwave dielectric ceramics is generally negative. Here, a novel m...

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Main Authors: Jiaqing Yang, Peng Lei, Xiaoqiang Song, Changzhi Yin, Meng Zhang, Weicheng Lei, Yiyang Cai, Mingfei Cheng, Yaodong Liu, Zihang Chen, Yaqing Hu, Wenzhong Lu, Wen Lei
Format: Article
Language:English
Published: Tsinghua University Press 2025-02-01
Series:Journal of Advanced Ceramics
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Online Access:https://www.sciopen.com/article/10.26599/JAC.2024.9221020
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author Jiaqing Yang
Peng Lei
Xiaoqiang Song
Changzhi Yin
Meng Zhang
Weicheng Lei
Yiyang Cai
Mingfei Cheng
Yaodong Liu
Zihang Chen
Yaqing Hu
Wenzhong Lu
Wen Lei
author_facet Jiaqing Yang
Peng Lei
Xiaoqiang Song
Changzhi Yin
Meng Zhang
Weicheng Lei
Yiyang Cai
Mingfei Cheng
Yaodong Liu
Zihang Chen
Yaqing Hu
Wenzhong Lu
Wen Lei
author_sort Jiaqing Yang
collection DOAJ
description The temperature coefficient of the resonant frequency (τf) of low-permittivity (εr) microwave dielectric ceramics is required to be near 0 ppm/°C for practical application. However, owing to the polarization mechanism, τf of low-εr microwave dielectric ceramics is generally negative. Here, a novel microwave dielectric ceramic, Ba3−xSrxMgSi2O8, with an abnormal positive τf at the applied temperature is presented. In this study, Sr2+ with a relatively small ionic radius was introduced to replace Ba2+, and a single-phase solid solution was formed (x > 0.5). Ba3−xSrxMgSi2O8 ceramics were discussed in glaserite-type topology with space groups of P3¯ for x ≤ 0.5, relatively high symmetry P3¯m1 for 0.5 < x < 2.5, and C2 for x ≥ 2.5. The εr peaks as a function of temperature initially shift to low temperatures and then return to high temperatures through an ion substitution strategy. Notably, remarkable microwave dielectric properties for BaSr2MgSi2O8 were observed: εr ≈ 14.2, Q×f ≈ 38,900 GHz, and τf ≈ +117 ppm/°C, which are superior to those of other low-εr silicate ceramics with positive τf values. Density functional theory simulation calculations revealed that the preferential occupation of Sr2+ ions could decrease the intrinsic formation energy and improve the microwave dielectric properties by mitigating the ionic size mismatch within the crystal structure. The present research offers a strategy for discovering novel microwave dielectric ceramics with abnormal τf values, which could serve as τf regulators in practical applications because of their low cost and excellent microwave dielectric properties.
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spelling doaj-art-ea3c85246f584c6f8bed67fcd0a99c2a2025-08-20T02:04:30ZengTsinghua University PressJournal of Advanced Ceramics2226-41082227-85082025-02-01142922102010.26599/JAC.2024.9221020Abnormal dielectric behavior of glaserite-type Ba3−xSrxMgSi2O8 solid solutionJiaqing Yang0Peng Lei1Xiaoqiang Song2Changzhi Yin3Meng Zhang4Weicheng Lei5Yiyang Cai6Mingfei Cheng7Yaodong Liu8Zihang Chen9Yaqing Hu10Wenzhong Lu11Wen Lei12School of Optical and Electronic Information, Key Lab of Functional Materials for Electronic Information (B) of MOE, Huazhong University of Science and Technology, Wuhan 430074, ChinaSchool of Optical and Electronic Information, Key Lab of Functional Materials for Electronic Information (B) of MOE, Huazhong University of Science and Technology, Wuhan 430074, ChinaWenzhou Key Laboratory of Microwave Communication Materials and Devices, Wenzhou Advanced Manufacturing Institute of HUST, Wenzhou 325035, ChinaWenzhou Key Laboratory of Microwave Communication Materials and Devices, Wenzhou Advanced Manufacturing Institute of HUST, Wenzhou 325035, ChinaSchool of Optical and Electronic Information, Key Lab of Functional Materials for Electronic Information (B) of MOE, Huazhong University of Science and Technology, Wuhan 430074, ChinaSchool of Optical and Electronic Information, Key Lab of Functional Materials for Electronic Information (B) of MOE, Huazhong University of Science and Technology, Wuhan 430074, ChinaSchool of Optical and Electronic Information, Key Lab of Functional Materials for Electronic Information (B) of MOE, Huazhong University of Science and Technology, Wuhan 430074, ChinaSchool of Optical and Electronic Information, Key Lab of Functional Materials for Electronic Information (B) of MOE, Huazhong University of Science and Technology, Wuhan 430074, ChinaSchool of Optical and Electronic Information, Key Lab of Functional Materials for Electronic Information (B) of MOE, Huazhong University of Science and Technology, Wuhan 430074, ChinaSchool of Optical and Electronic Information, Key Lab of Functional Materials for Electronic Information (B) of MOE, Huazhong University of Science and Technology, Wuhan 430074, ChinaSchool of Optical and Electronic Information, Key Lab of Functional Materials for Electronic Information (B) of MOE, Huazhong University of Science and Technology, Wuhan 430074, ChinaSchool of Optical and Electronic Information, Key Lab of Functional Materials for Electronic Information (B) of MOE, Huazhong University of Science and Technology, Wuhan 430074, ChinaSchool of Optical and Electronic Information, Key Lab of Functional Materials for Electronic Information (B) of MOE, Huazhong University of Science and Technology, Wuhan 430074, ChinaThe temperature coefficient of the resonant frequency (τf) of low-permittivity (εr) microwave dielectric ceramics is required to be near 0 ppm/°C for practical application. However, owing to the polarization mechanism, τf of low-εr microwave dielectric ceramics is generally negative. Here, a novel microwave dielectric ceramic, Ba3−xSrxMgSi2O8, with an abnormal positive τf at the applied temperature is presented. In this study, Sr2+ with a relatively small ionic radius was introduced to replace Ba2+, and a single-phase solid solution was formed (x > 0.5). Ba3−xSrxMgSi2O8 ceramics were discussed in glaserite-type topology with space groups of P3¯ for x ≤ 0.5, relatively high symmetry P3¯m1 for 0.5 < x < 2.5, and C2 for x ≥ 2.5. The εr peaks as a function of temperature initially shift to low temperatures and then return to high temperatures through an ion substitution strategy. Notably, remarkable microwave dielectric properties for BaSr2MgSi2O8 were observed: εr ≈ 14.2, Q×f ≈ 38,900 GHz, and τf ≈ +117 ppm/°C, which are superior to those of other low-εr silicate ceramics with positive τf values. Density functional theory simulation calculations revealed that the preferential occupation of Sr2+ ions could decrease the intrinsic formation energy and improve the microwave dielectric properties by mitigating the ionic size mismatch within the crystal structure. The present research offers a strategy for discovering novel microwave dielectric ceramics with abnormal τf values, which could serve as τf regulators in practical applications because of their low cost and excellent microwave dielectric properties.https://www.sciopen.com/article/10.26599/JAC.2024.9221020microwave dielectric ceramicsabnormal dielectric behaviorion size mismatch[sio4] tetrahedra tiltingphase transitiondensity functional theory (dft)
spellingShingle Jiaqing Yang
Peng Lei
Xiaoqiang Song
Changzhi Yin
Meng Zhang
Weicheng Lei
Yiyang Cai
Mingfei Cheng
Yaodong Liu
Zihang Chen
Yaqing Hu
Wenzhong Lu
Wen Lei
Abnormal dielectric behavior of glaserite-type Ba3−xSrxMgSi2O8 solid solution
Journal of Advanced Ceramics
microwave dielectric ceramics
abnormal dielectric behavior
ion size mismatch
[sio4] tetrahedra tilting
phase transition
density functional theory (dft)
title Abnormal dielectric behavior of glaserite-type Ba3−xSrxMgSi2O8 solid solution
title_full Abnormal dielectric behavior of glaserite-type Ba3−xSrxMgSi2O8 solid solution
title_fullStr Abnormal dielectric behavior of glaserite-type Ba3−xSrxMgSi2O8 solid solution
title_full_unstemmed Abnormal dielectric behavior of glaserite-type Ba3−xSrxMgSi2O8 solid solution
title_short Abnormal dielectric behavior of glaserite-type Ba3−xSrxMgSi2O8 solid solution
title_sort abnormal dielectric behavior of glaserite type ba3 xsrxmgsi2o8 solid solution
topic microwave dielectric ceramics
abnormal dielectric behavior
ion size mismatch
[sio4] tetrahedra tilting
phase transition
density functional theory (dft)
url https://www.sciopen.com/article/10.26599/JAC.2024.9221020
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