The structure evolution and origin of ultrahigh dielectric properties have been investigated in the low temperature range from 300 K to 5 K for [001]-oriented 0.68 Pb(Mg_(1/3)Nb_(2/3))O_3–0.33PbTiO_3(PMN–33 PT) crys...The structure evolution and origin of ultrahigh dielectric properties have been investigated in the low temperature range from 300 K to 5 K for [001]-oriented 0.68 Pb(Mg_(1/3)Nb_(2/3))O_3–0.33PbTiO_3(PMN–33 PT) crystal. The experimental results reveal that a short-range ordered monoclinic MAis the dominant phase at ambient temperature. As the temperature drops below 270 K, the MAtransforms into monoclinic MC, and the MCremains stable until 5 K. Although no phase transition occurs from 5 K to 245 K, polar nanoregions(PNRs) display visible changes. The instability of PNRs is suggested as responsible for the low temperature relaxation. The ultrahigh dielectric constant at room temperature is associated with the instability of local structure and phase transition. Our research provides an insight into the design of high-performance ferroelectric materials.展开更多
A systematic investigation of the Li2Ti1-x(Mg_(1/3)Nb_(2/3))xO_(3)(0.1≤x≤0.35)solid solutions synthesized by traditional solid-state reaction method is reported in this work.In the composition range of 0.1≤x≤0.25,...A systematic investigation of the Li2Ti1-x(Mg_(1/3)Nb_(2/3))xO_(3)(0.1≤x≤0.35)solid solutions synthesized by traditional solid-state reaction method is reported in this work.In the composition range of 0.1≤x≤0.25,a monoclinic rock salt structured solid solution was formed.When x increased to 0.3,a phase transition from monoclinic to cubic phase,along with an order-disorder phase transition,was observed.With x increased from 0.1 to 0.35,the microwave permittivity(εr)and temperature coefficient of resonant frequency(TCF)of the Li2Ti1-x(Mg_(1/3)Nb_(2/3))xO_(3)ceramics decreased linearly from 21.0 to 18.6,+27.1 to-19.4 ppm/℃,respectively.The Li_(2)Ti_(0.75)(Mg_(1/3)Nb_(2/3))0.25O_(3)ceramic sintered at 1170℃shows high performance of microwave dielectric properties with aεr~19.6,a Qf(Q=quality factor=1/dielectric loss;f=resonant frequency)~109,770 GHz(at 7.7 GHz)and a near zero TCF~t 1.2 ppm/℃.Moreover,the burying sintering process can reduce the volatilization of lithium so that the porosity of Li_(2)Ti_(0.75)(Mg_(1/3)Nb_(2/3))0.25O_(3)ceramic was reduced effectively,which made Li_(2)Ti_(0.75)(Mg_(1/3)Nb_(2/3))0.25O_(3)ceramic promising for future applications.Selected area electron diffraction patterns,high-resolution transmission electron microscopy,Raman and far-infrared spectra were employed to study the relation between crystal structure and microwave dielectric properties in detail.展开更多
Non-stoichiometric Nd_((1+x))(Mg_(1/2)Sn_(1/2))O_(3)(-0.04=x≤0.04,NMS)ceramics were fabricated via a conventional solid-state reaction method.Crystal structures and morphologies were investigated by Xray diffraction(...Non-stoichiometric Nd_((1+x))(Mg_(1/2)Sn_(1/2))O_(3)(-0.04=x≤0.04,NMS)ceramics were fabricated via a conventional solid-state reaction method.Crystal structures and morphologies were investigated by Xray diffraction(XRD)and scanning electron microscopy(SEM),respectively.The main crystalline phase is monoclinic Nd(Mg_(1/2)Sn_(1/2))O_(3) with a double perovskite structure(P21/n space group)for the NMS system proved by XRD.The sample at x=0.01 has the best crystallinity and evenly distributed crystal grains observed by SEM.The optimum performances(ε_(r)=19.87,Q×f=41840 GHz,f=12.05 GHz)are obtained at x=0.01.Lattice vibrational modes of the Raman spectra were assigned and illustrated,in detail.The dielectric properties obtained by fitting infrared reflectance spectra with the help of four-parameter semi-quantum model are consistent with the calculated values by microscopic polarization and damping coefficients.The reverse translational vibration of the NdeMgO_(6),the F_(5u)^((5)) mode,provides the greatest contribution to the dielectric response.The relationships between crystal structures and dielectric properties were mainly established using lattice vibrational modes as a media.展开更多
Sr_(2)MgWO_(6)(SMW)is a typical perovskite oxide compound,but there has been little research on the effects of processing on its dielectric properties.In this work,SMW ceramics were prepared by solid-state synthesis w...Sr_(2)MgWO_(6)(SMW)is a typical perovskite oxide compound,but there has been little research on the effects of processing on its dielectric properties.In this work,SMW ceramics were prepared by solid-state synthesis with sintering at 1450℃,1475℃,1500℃and 1525℃,respectively.XRD results confirmed that the samples possessed double perovskite structure(Fm-3m).The Raman and FTIR spectra were used to study the lattice vibrational modes.The FPSQ model was used to obtain the fitting curves of the FTIR spectra and derive the intrinsic properties of the material that were found to be in agreement with the measured data.The structure-property relationships were successfully established based on the Raman mode results.The optimal sintering temperature of SMW ceramics was identified as 1475℃due to the excellent performances characteristics(ε_(r)=16.97,Q×f=23,872 GHz,τ_(f)=-35.38 ppm/℃)obtained at this temperature.This study explored the relationships among the crystal structures,lattice vibrational characteristics and dielectric properties of SMW ceramics,so as to further understand their dielectric response mechanism and lay a solid theoretical foundation for the development of microwave ceramics.展开更多
A low-dimensional ion-pair compound[4-CN-Bz-4-Ph-Py][Ni(mnt)2](1,4-CN-Bz-4-Ph-Py=(4’-cyanobenzyl)-4-phenylpridinium)and mnt^2-=maleonitriledithiolate)was designed and synthesized.The cations and anions of 1 formed ir...A low-dimensional ion-pair compound[4-CN-Bz-4-Ph-Py][Ni(mnt)2](1,4-CN-Bz-4-Ph-Py=(4’-cyanobenzyl)-4-phenylpridinium)and mnt^2-=maleonitriledithiolate)was designed and synthesized.The cations and anions of 1 formed irregular segregated stacks along the a axis.1 exhibits weak paramagnetism over the temperature range of 2~300 K.The dielectric constant of compound 1 is between 2.75 and 5.55 from 30 to 140℃.1 is a very rare metal-bis-dithiolene complex with very low dielectric constant in high temperature.Our results will shed light on the design and preparation of new multi-functional molecular materials combining magnetic and dielectric properties.展开更多
The paper reports results on the complex study on ferroelectric ceramics that represent solid solutions containing components with a perovskite-type or columbite-type structure.Solid solutions of a three-component(1−x...The paper reports results on the complex study on ferroelectric ceramics that represent solid solutions containing components with a perovskite-type or columbite-type structure.Solid solutions of a three-component(1−x−y)NaNbO_(3)−xKNbO_(3)−yCdNb_(2)O_(6) system are manufactured at x=0.05-0.20 and y=0.10.Domain structures in ceramic grains are studied.The consistency between experimental and calculated results is examined for coexisting phases split into non-180°domains(mechanical twins)in the solid solution with x=0.15.A correlation between the internal structure(crystal,domain,granular,and defect)and fundamental electromechanical and polarization properties is stated for the studied three-component solid solutions.展开更多
Ce2[Zr_(1-x)(Mg_(1/3)Sb_(2/3))_(x)]_(3)(MoO_(4))_(9)(0.02≤x≤0.10)ceramics were prepared by the traditional solid-state method.A single phase,belonging to the space group of R3c,was detected by using X-ray diffractio...Ce2[Zr_(1-x)(Mg_(1/3)Sb_(2/3))_(x)]_(3)(MoO_(4))_(9)(0.02≤x≤0.10)ceramics were prepared by the traditional solid-state method.A single phase,belonging to the space group of R3c,was detected by using X-ray diffraction at the sintering temperatures ranging from 700 to 850℃.The microstructures of samples were examined by applying scanning electron microscopy(SEM).The crystal structure refinement of these samples was investigated in detail by performing the Rietveld refinement method.The intrinsic properties were calculated and explored via far-infrared reflectivity spectroscopy.The correlations between the chemical bond parameters and microwave dielectric properties were calculated and analyzed by Phillips-van Vechten-Levine(P-V-L)theory.Ce_(2)[Zr_(0.94)(Mg_(1/3)Sb_(2/3))_(0.06)]_(3)(Mo0_(4))_(9)ceramics with excellent dielectric properties were sintered at 725℃for 6 h(εr=10.37,Q×f=71,748 GHz,andτf=-13.6 ppm/℃,εr is the dielectric constant,τf is the quality factor,and rf is the temperature coefficient of resonant frequency).展开更多
基金Project supported by the National Natural Science Foundation of China(Grant Nos.51602242 and 51472197)the Natural Science Basic Research Plan in Shaanxi Province of China(Grant No.2018JM5097)
文摘The structure evolution and origin of ultrahigh dielectric properties have been investigated in the low temperature range from 300 K to 5 K for [001]-oriented 0.68 Pb(Mg_(1/3)Nb_(2/3))O_3–0.33PbTiO_3(PMN–33 PT) crystal. The experimental results reveal that a short-range ordered monoclinic MAis the dominant phase at ambient temperature. As the temperature drops below 270 K, the MAtransforms into monoclinic MC, and the MCremains stable until 5 K. Although no phase transition occurs from 5 K to 245 K, polar nanoregions(PNRs) display visible changes. The instability of PNRs is suggested as responsible for the low temperature relaxation. The ultrahigh dielectric constant at room temperature is associated with the instability of local structure and phase transition. Our research provides an insight into the design of high-performance ferroelectric materials.
基金the National Key Research and Development Program of China(2017YFB0406301)the Young Star Project of Science and Technology of Shaanxi Province(2016KJXX-34)+1 种基金the Fundamental Research Funds for the Central University,and the 111 Project of China(B14040)The SEM and TEM work was done at the International Center for Dielectric Research(ICDR),Xi'an Jiaotong University,Xi'an,China and the authors thank Ms.Yan-Zhu Dai and Mr Chuan-Sheng Ma for their help in using SEM and TEM.
文摘A systematic investigation of the Li2Ti1-x(Mg_(1/3)Nb_(2/3))xO_(3)(0.1≤x≤0.35)solid solutions synthesized by traditional solid-state reaction method is reported in this work.In the composition range of 0.1≤x≤0.25,a monoclinic rock salt structured solid solution was formed.When x increased to 0.3,a phase transition from monoclinic to cubic phase,along with an order-disorder phase transition,was observed.With x increased from 0.1 to 0.35,the microwave permittivity(εr)and temperature coefficient of resonant frequency(TCF)of the Li2Ti1-x(Mg_(1/3)Nb_(2/3))xO_(3)ceramics decreased linearly from 21.0 to 18.6,+27.1 to-19.4 ppm/℃,respectively.The Li_(2)Ti_(0.75)(Mg_(1/3)Nb_(2/3))0.25O_(3)ceramic sintered at 1170℃shows high performance of microwave dielectric properties with aεr~19.6,a Qf(Q=quality factor=1/dielectric loss;f=resonant frequency)~109,770 GHz(at 7.7 GHz)and a near zero TCF~t 1.2 ppm/℃.Moreover,the burying sintering process can reduce the volatilization of lithium so that the porosity of Li_(2)Ti_(0.75)(Mg_(1/3)Nb_(2/3))0.25O_(3)ceramic was reduced effectively,which made Li_(2)Ti_(0.75)(Mg_(1/3)Nb_(2/3))0.25O_(3)ceramic promising for future applications.Selected area electron diffraction patterns,high-resolution transmission electron microscopy,Raman and far-infrared spectra were employed to study the relation between crystal structure and microwave dielectric properties in detail.
基金supported by National Natural Science Foundation of China(Grant 11874240)Guangxi Information Materials Key Laboratory Open Research Fund(171007-K)+3 种基金State Key Laboratory of New Ceramic and Fine Processing Tsinghua University(No.KF201811)the Opening Project of Key Laboratory of Inorganic Functional Materials and Devices,Chinese Academy of Sciences(Grant No.KLIFMD201803)the Natural Science Foundation of Shandong Province,China(No.ZR2016EMM21)Scientific Research Foundation of Shandong University of Science and Technology for Recruited Talents(No.2016RCJJ002).
文摘Non-stoichiometric Nd_((1+x))(Mg_(1/2)Sn_(1/2))O_(3)(-0.04=x≤0.04,NMS)ceramics were fabricated via a conventional solid-state reaction method.Crystal structures and morphologies were investigated by Xray diffraction(XRD)and scanning electron microscopy(SEM),respectively.The main crystalline phase is monoclinic Nd(Mg_(1/2)Sn_(1/2))O_(3) with a double perovskite structure(P21/n space group)for the NMS system proved by XRD.The sample at x=0.01 has the best crystallinity and evenly distributed crystal grains observed by SEM.The optimum performances(ε_(r)=19.87,Q×f=41840 GHz,f=12.05 GHz)are obtained at x=0.01.Lattice vibrational modes of the Raman spectra were assigned and illustrated,in detail.The dielectric properties obtained by fitting infrared reflectance spectra with the help of four-parameter semi-quantum model are consistent with the calculated values by microscopic polarization and damping coefficients.The reverse translational vibration of the NdeMgO_(6),the F_(5u)^((5)) mode,provides the greatest contribution to the dielectric response.The relationships between crystal structures and dielectric properties were mainly established using lattice vibrational modes as a media.
基金supported by National Natural Science Foundation of China(Grant 11874240)Shandong Provincial Key Research and Development Program,China(No.2019GGX101060).
文摘Sr_(2)MgWO_(6)(SMW)is a typical perovskite oxide compound,but there has been little research on the effects of processing on its dielectric properties.In this work,SMW ceramics were prepared by solid-state synthesis with sintering at 1450℃,1475℃,1500℃and 1525℃,respectively.XRD results confirmed that the samples possessed double perovskite structure(Fm-3m).The Raman and FTIR spectra were used to study the lattice vibrational modes.The FPSQ model was used to obtain the fitting curves of the FTIR spectra and derive the intrinsic properties of the material that were found to be in agreement with the measured data.The structure-property relationships were successfully established based on the Raman mode results.The optimal sintering temperature of SMW ceramics was identified as 1475℃due to the excellent performances characteristics(ε_(r)=16.97,Q×f=23,872 GHz,τ_(f)=-35.38 ppm/℃)obtained at this temperature.This study explored the relationships among the crystal structures,lattice vibrational characteristics and dielectric properties of SMW ceramics,so as to further understand their dielectric response mechanism and lay a solid theoretical foundation for the development of microwave ceramics.
基金supported by the Natural Science Foundation of Jiangsu Province and Natural Science Training Foundation of Nanjing Xiaozhuang University(Nos.BK20171125 and 2016NXY12)
文摘A low-dimensional ion-pair compound[4-CN-Bz-4-Ph-Py][Ni(mnt)2](1,4-CN-Bz-4-Ph-Py=(4’-cyanobenzyl)-4-phenylpridinium)and mnt^2-=maleonitriledithiolate)was designed and synthesized.The cations and anions of 1 formed irregular segregated stacks along the a axis.1 exhibits weak paramagnetism over the temperature range of 2~300 K.The dielectric constant of compound 1 is between 2.75 and 5.55 from 30 to 140℃.1 is a very rare metal-bis-dithiolene complex with very low dielectric constant in high temperature.Our results will shed light on the design and preparation of new multi-functional molecular materials combining magnetic and dielectric properties.
基金support of the Ministry of Science and Higher Education of the Russian Federation(State Task in the Field of Scientific Activity,Scientific Project No.0852-2020-0032/BAZ0110/20-3-07IF).
文摘The paper reports results on the complex study on ferroelectric ceramics that represent solid solutions containing components with a perovskite-type or columbite-type structure.Solid solutions of a three-component(1−x−y)NaNbO_(3)−xKNbO_(3)−yCdNb_(2)O_(6) system are manufactured at x=0.05-0.20 and y=0.10.Domain structures in ceramic grains are studied.The consistency between experimental and calculated results is examined for coexisting phases split into non-180°domains(mechanical twins)in the solid solution with x=0.15.A correlation between the internal structure(crystal,domain,granular,and defect)and fundamental electromechanical and polarization properties is stated for the studied three-component solid solutions.
基金supported by the National Natural Science Foundation(No.51972143).
文摘Ce2[Zr_(1-x)(Mg_(1/3)Sb_(2/3))_(x)]_(3)(MoO_(4))_(9)(0.02≤x≤0.10)ceramics were prepared by the traditional solid-state method.A single phase,belonging to the space group of R3c,was detected by using X-ray diffraction at the sintering temperatures ranging from 700 to 850℃.The microstructures of samples were examined by applying scanning electron microscopy(SEM).The crystal structure refinement of these samples was investigated in detail by performing the Rietveld refinement method.The intrinsic properties were calculated and explored via far-infrared reflectivity spectroscopy.The correlations between the chemical bond parameters and microwave dielectric properties were calculated and analyzed by Phillips-van Vechten-Levine(P-V-L)theory.Ce_(2)[Zr_(0.94)(Mg_(1/3)Sb_(2/3))_(0.06)]_(3)(Mo0_(4))_(9)ceramics with excellent dielectric properties were sintered at 725℃for 6 h(εr=10.37,Q×f=71,748 GHz,andτf=-13.6 ppm/℃,εr is the dielectric constant,τf is the quality factor,and rf is the temperature coefficient of resonant frequency).
