Bi_(1-x)Ho_(x)VO_(4)(0.1≤x≤0.9)ceramics were prepared via a solid-state reaction method,and all the ceram-ics could be well densified in the 920–980℃range.The ceramics with 0.1≤x<0.4 were composed of both mono...Bi_(1-x)Ho_(x)VO_(4)(0.1≤x≤0.9)ceramics were prepared via a solid-state reaction method,and all the ceram-ics could be well densified in the 920–980℃range.The ceramics with 0.1≤x<0.4 were composed of both monoclinic scheelite(M)and tetragonal zircon(T)phases,and a single M phase could be obtained in the range of x≥0.4.The measuredε_(r) decreased from 58.9(x=0.1)to 14.7(x=0.9),so do the calcu-lated values(ε_(r)(C−M)=34.3–12.1),and the main reason forε_(r)>ε_(r)(C−M)was the rattling of Ho^(3+)in the dodecahedron.Two points with zeroτf appeared in Bi1–x Hox VO4(0≤x≤1)ceramics,and the best mi-crowave dielectric properties withε_(r)=16.6,Q×f=18,400 GHz(f=10.69 GHz),andτf=+3.29 ppm/℃were obtained in the Bi_(0.2)Ho_(0.8)VO_(4)ceramic.The change in temperature coefficient of ionic polarizability(τ_(αm))caused by the rattling effect of cations is the physical essence that affectsτf.Therefore,the rattling effect can be used as an effective mechanism to regulateτf in low-ε_(r) materials.Furthermore,there was no chemical reaction between Bi_(1-x)Ho_(x)VO_(4) and Ag electrode,which indicates potential applications in low-temperature co-fired ceramic(LTCC)technology.展开更多
Dielectric ceramics with low permittivity(ε_(r)),high quality factor(Q×f),and near-zero resonant frequency(τ_(f))in the microwave bands are key materials used in fifth/sixth-generation(5G/6G)telecommunication,w...Dielectric ceramics with low permittivity(ε_(r)),high quality factor(Q×f),and near-zero resonant frequency(τ_(f))in the microwave bands are key materials used in fifth/sixth-generation(5G/6G)telecommunication,whileτ_(f) of most low-εr microwave dielectric ceramics is relatively negative.In this work,the first low-εr Ga-based ceramic SrGa_(12_O_(19) with an anomalous positiveτ_(f) was reported,and the causes of the positiveτ_(f),intrinsic polarization,and loss mechanism were systematically studied.X-ray diffraction(XRD)and transmission electron microscopy(TEM)revealed that the SrGa_(12_O_(19) ceramic formed a pure hexagonal magnetoplumbite structure with spinel blocks and rock-salt blocks stacked along the crystallographic c-axis.When sintered at 1430℃,it possessed the optimal microwave dielectric properties of a lowεr of 14.46,high Q×f of 64,705 GHz,and exceptional positiveτ_(f) of+55.7 ppm/℃,along with a low linear thermal expansion coefficient(αL)of 11.617 ppm/℃.The large positive deviation betweenεr andεr(C–M)of 45.31%resulted from the rattling effect of atoms in the rock-salt block.The unique positiveτ_(f)(+55.7 ppm/℃)was governed by the rattling effect,resulting in a positiveταm(the temperature coefficient of ion polarizability)of 8.489 ppm/℃ and a large negative temperature coefficient of permittivity(τε)of−132.864 ppm/℃.Phillips–Vechten–Levine(P–V–L)chemical bond theory revealed greater contributions of the spinel block to bond ionicity(fi,52.95%),permittivity(ε,55.15%),bond energy(E,56.87%),and lattice energy(U,74.88%)than those of the rock-salt block.The intrinsic dielectric properties were analyzed using infrared(IR)reflectivity spectra.The favorable performance of the SrGa_(12)O_(19) ceramic indicated that it is a novelτ_(f) compensator.This selection of compounds with different structural layer combinations provides a new idea for exploring excellent microwave dielectric ceramics.展开更多
We prepared (1-x)CaTiO3-xLaAlO3 (0 ≤x≤ 1) microwave dielectric ceramics using a conventional two-step solid-state reaction method,and investigated microwave dielectric properties of the ceramics in terms of A/B-site...We prepared (1-x)CaTiO3-xLaAlO3 (0 ≤x≤ 1) microwave dielectric ceramics using a conventional two-step solid-state reaction method,and investigated microwave dielectric properties of the ceramics in terms of A/B-site ionic-parameters.Ionic-parameters such as ionic polarizability,A-site bond valence,and ionic rattling were linked to the microwave dielectric properties.As the LaAlO3 content x in the (1-x)CaTiO3-xLaAlO3 ceramics increased from 0.3 to 0.7,the dielectric constant gradually decreased,which was attributed to the decrease of polarizability deviation and suppression of the cation rattling.The temperature coefficient of the resonant frequency decreased as the content of LaAlO3 increased because of the increase of A-site cation bond valence.The quality factor value (Q × f) increased as LaAlO3 content increased because of the enhancement of the order degree of B-site cation.A significant deterioration of the temperature coefficient of the resonant frequency and Q ×fvalue was observed at the composition x =0.5.These decreases were attributed to a phase transition from orthorhombic crystal (for x ≤ 0.5) to rhombohedral crystal (for x ＞ 0.5).展开更多
基金supported by the Natural Science Foundation of Guangxi Zhuang Autonomous Region(No.2023GXNSFBA026076)the Guangxi Key Laboratory of Optical and Electronic Materials and Devices(No.22KF-10)+1 种基金the Natural Science Foundation of China(Nos.21965009 and 22105048)the Guilin University of Technology Research Startup Project(No.GUTQDJJ2021073),and the Guangxi BaGui Scholars Special Funding.
文摘Bi_(1-x)Ho_(x)VO_(4)(0.1≤x≤0.9)ceramics were prepared via a solid-state reaction method,and all the ceram-ics could be well densified in the 920–980℃range.The ceramics with 0.1≤x<0.4 were composed of both monoclinic scheelite(M)and tetragonal zircon(T)phases,and a single M phase could be obtained in the range of x≥0.4.The measuredε_(r) decreased from 58.9(x=0.1)to 14.7(x=0.9),so do the calcu-lated values(ε_(r)(C−M)=34.3–12.1),and the main reason forε_(r)>ε_(r)(C−M)was the rattling of Ho^(3+)in the dodecahedron.Two points with zeroτf appeared in Bi1–x Hox VO4(0≤x≤1)ceramics,and the best mi-crowave dielectric properties withε_(r)=16.6,Q×f=18,400 GHz(f=10.69 GHz),andτf=+3.29 ppm/℃were obtained in the Bi_(0.2)Ho_(0.8)VO_(4)ceramic.The change in temperature coefficient of ionic polarizability(τ_(αm))caused by the rattling effect of cations is the physical essence that affectsτf.Therefore,the rattling effect can be used as an effective mechanism to regulateτf in low-ε_(r) materials.Furthermore,there was no chemical reaction between Bi_(1-x)Ho_(x)VO_(4) and Ag electrode,which indicates potential applications in low-temperature co-fired ceramic(LTCC)technology.
基金funded by the Natural Science Foundation of Guangxi Zhuang Autonomous Region(No.2024GXNSFFA010013)the Project of Scientific Research and Technical Exploitation Program of the Guangxi Zhuang Autonomous Region(No.AD24010021)+1 种基金the Guilin University of Technology Research Startup Project(No.GUTQDJJ2019183)Guangxi BaGui Scholars Special Funding。
文摘Dielectric ceramics with low permittivity(ε_(r)),high quality factor(Q×f),and near-zero resonant frequency(τ_(f))in the microwave bands are key materials used in fifth/sixth-generation(5G/6G)telecommunication,whileτ_(f) of most low-εr microwave dielectric ceramics is relatively negative.In this work,the first low-εr Ga-based ceramic SrGa_(12_O_(19) with an anomalous positiveτ_(f) was reported,and the causes of the positiveτ_(f),intrinsic polarization,and loss mechanism were systematically studied.X-ray diffraction(XRD)and transmission electron microscopy(TEM)revealed that the SrGa_(12_O_(19) ceramic formed a pure hexagonal magnetoplumbite structure with spinel blocks and rock-salt blocks stacked along the crystallographic c-axis.When sintered at 1430℃,it possessed the optimal microwave dielectric properties of a lowεr of 14.46,high Q×f of 64,705 GHz,and exceptional positiveτ_(f) of+55.7 ppm/℃,along with a low linear thermal expansion coefficient(αL)of 11.617 ppm/℃.The large positive deviation betweenεr andεr(C–M)of 45.31%resulted from the rattling effect of atoms in the rock-salt block.The unique positiveτ_(f)(+55.7 ppm/℃)was governed by the rattling effect,resulting in a positiveταm(the temperature coefficient of ion polarizability)of 8.489 ppm/℃ and a large negative temperature coefficient of permittivity(τε)of−132.864 ppm/℃.Phillips–Vechten–Levine(P–V–L)chemical bond theory revealed greater contributions of the spinel block to bond ionicity(fi,52.95%),permittivity(ε,55.15%),bond energy(E,56.87%),and lattice energy(U,74.88%)than those of the rock-salt block.The intrinsic dielectric properties were analyzed using infrared(IR)reflectivity spectra.The favorable performance of the SrGa_(12)O_(19) ceramic indicated that it is a novelτ_(f) compensator.This selection of compounds with different structural layer combinations provides a new idea for exploring excellent microwave dielectric ceramics.
文摘We prepared (1-x)CaTiO3-xLaAlO3 (0 ≤x≤ 1) microwave dielectric ceramics using a conventional two-step solid-state reaction method,and investigated microwave dielectric properties of the ceramics in terms of A/B-site ionic-parameters.Ionic-parameters such as ionic polarizability,A-site bond valence,and ionic rattling were linked to the microwave dielectric properties.As the LaAlO3 content x in the (1-x)CaTiO3-xLaAlO3 ceramics increased from 0.3 to 0.7,the dielectric constant gradually decreased,which was attributed to the decrease of polarizability deviation and suppression of the cation rattling.The temperature coefficient of the resonant frequency decreased as the content of LaAlO3 increased because of the increase of A-site cation bond valence.The quality factor value (Q × f) increased as LaAlO3 content increased because of the enhancement of the order degree of B-site cation.A significant deterioration of the temperature coefficient of the resonant frequency and Q ×fvalue was observed at the composition x =0.5.These decreases were attributed to a phase transition from orthorhombic crystal (for x ≤ 0.5) to rhombohedral crystal (for x ＞ 0.5).
