We measure the colossal permittivity in single crystal Fe$_2$TiO$_5$ using broadband spectroscopy in the frequency range 20 Hz - 1 MHz. The relaxation response is analyzed using a Debye-like model with Arrhenius activation in two different ways and yields an energy barrier of 286.1 $\pm$ 2.8 meV. DC transport yields an activation energy of 288.8 $\pm$ 2.8 meV. These results strongly imply that the energy barrier for localized dipole motion and itinerant charge transport originate from the same atom-level forces. A further implication is that colossal dielectric behavior is a microscopic bulk phenomenon arising from a system on brink of metallicity.
Comments on "Giant Dielectric Response in the One-Dimensional Charge-Ordered Semiconductor (NbSe_{4})_{3}I" and "Colossal Magnetocapacitance and Colossal Magnetoresistance in HgCr_{2}S_{4}"
对“一维电荷有序半导体（NbSe_{4}）_{3}I中的巨介电响应”（D. Staresinic等人，物理修订版信函96，046402（2006））和“Colossal Magnetocapacitance and Colossal Magnetoresistance in HgCr_{2} S_{4}“（S. Weber等人，物理修订信函157202（2006））
Recently, materials exhibiting colossal dielectric constant ($CDC$) have attracted significant attention because of their high dielectric constant and potential applications in electronic devices, such as high dielectric capacitors, capacitor sensors, random access memories and so on.
Electrical conductivity and high dielectric constant are in principle self-excluding, which makes the terms insulator and dielectric usually synonymous. This is certainly true when the electrical carriers are electrons, but not necessarily in a material where ions are extremely mobile, electronic conduction is negligible and the charge transfer at the interface is immaterial. Here we demonstrate in a perovskite-derived structure containing five-coordinated Ti atoms, a colossal dielectric constant (up to $\mbox{10}^9$) together with very high ionic conduction $\mbox{10}^{-3}\mbox{S.cm}^{-1}$ at…
The development of dielectric materials with colossal permittivity is important for the miniaturization of electronic devices and fabrication of high-density energy-storage devices. The electron-pinned defect-dipoles has been recently proposed to boost the permittivity of (Nb + In) co-doped TiO2 to 105. However, the follow-up studies suggest an extrinsic contribution to the colossal permittivity from thermally excited carriers. Herein, we demonstrate a marked enhancement in the permittivity of (Nb + In) co-doped TiO2 single crystals at sufficiently low temperatures such that the thermally exci…
REPLY to Comments on "Giant Dielectric Response in the One-Dimensional Charge-Ordered Semiconductor (NbSe4)3I" and "Colossal Magnetocapacitance and Colossal Magnetoresistance in HgCr2S4" (cond-mat/0607500)
A colossal dielectric response of Bi1-xSmxFeO3 nanopowders
Institute of Physics, National Academy of Sciences of Ukraine（乌克兰国家科学院物理研究所）；Taras Shevchenko National University of Kyiv（基辅塔拉斯舍甫琴科国立大学）；Stockholm University, Department of Chemistry（斯德哥尔摩大学化学系）；University of Ukraine “Igor Sikorsky Kyiv Polytechnic Institute”（乌克兰伊戈尔·西科尔斯基基辅理工学院）；Frantsevich Institute for Problems in Materials Science of the National Academy of Sciences of Ukraine（乌克兰国家科学院弗朗采维奇材料科学问题研究所）
In the present work we demonstrate that in addition to the well-known colossal-dielectric-constant material CaCu3Ti4O12 also various members of the series Ln2/3Cu3Ti4O12 with Ln = La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er and Tm, exhibit giant values of the dielectric constant. Just as CaCu3Ti4O12, all these materials show a Maxwell-Wagner type relaxation process. For the best material, Pr2/3Cu3Ti4O12, we provide a detailed investigation of its dielectric properties in a broad frequency range up to 1 GHz. Polarization at internal barriers, most likely grain boundaries, seems to be the reason …
We report magnetic, dielectric and magnetodielectric responses of pure monoclinic bulk phase of partially-disordered La2NiMnO6, exhibiting a spectrum of unusual properties and establish that this system intrinsically is a true multiglass with a large magnetodielectric coupling (8-20%) over a wide range of temperatures (150 - 300 K). Specifically, our results establish a unique way to obtain colossal magnetodielectricity, independent of any striction effects, by engineering the asymmetric hopping contribution to the dielectric constant via the tuning of the relative spin orientations between ne…
We calculate the lattice dielectric function of strongly anharmonic rutile $\mathrm{TiO}_2$ from ab initio anharmonic lattice dynamics methods. Since an accurate calculation of the $Γ$ point phonons is essential for determining optical properties, we employ the modified self-consistent approach, including third-order anharmonicity as well as fourth-order anharmonicity. The resulting optical phonon frequencies and linewidths at the $Γ$ point much better agree with experimental measurements than those from a perturbative approach. We show that the four-phonon scattering process contributes as mu…
We study the temperature-dependent evolution of the octahedral tilt order in a lead-free relaxor ferroelectric and its impact on the ferroelectric properties. Using diffuse neutron scattering on a 0.964Na$_{1/2}$Bi$_{1/2}$TiO$_3$-0.036BaTiO$_3$ single crystal, we suggest a model for the temperature-dependent nanostructure of this perovskite that features chemically pinned tetragonal platelets embedded in the rhombohedral matrix, often separated by a cubic intermediate phase. Our results show a clear correlation between the squared thickness of the tetragonal platelets and the dielectric permit…
Dielectric permittivity was studied in ceramics of relaxor ferroelectric bismuth-sodium titanate Na$_{0.5}$Bi$_{0.5}$TiO$_{3}$. The measurements were performed on as sintered and heat treated in vacuum samples. The diffuse dielectric anomalies associated with the structural phase transitions were observed in as sintered samples. The intense peak of permittivity ($ \varepsilon_{\text{max}} \sim 10^{4}$) appeared after heat treating in vacuum. The anomaly of $\varepsilon(T)$ was contributed by slow polarization processes ($f<10$ kHz) and was non-stable, vanishing on heating in air up to $\sim 80…
Entropic contributions to the stability of solids are very well understood and the mixing entropy has been used for forming various solids, for instance such as inverse spinels. A particular development was related to high entropy alloys in which the configurational disorder is responsible for forming simple solid solutions and which are thoroughly studied for various applications especially due to their mechanical properties but also electrical properties, hydrogen storage, magnetic properties. Many unexplored compositions and properties still remain for this class of materials due to their l…
The structural, dielectric and ferroelectric properties of lead-free (Na0.5-xKxBi0.5-xLax)TiO3 powders synthesized by sol-gel self-combustion method were investigated. Rietveld refinement of Synchrotron x-ray diffraction data confirms pure single phase rhombohedral crystal structure with R3c space group for all the compositions and anti-phase octahedral tilting angle decreased with increase in composition x. Homogeneity and elemental proportions were confirmed by Energy dispersive x-ray spectrometry. The temperature-dependent dielectric study has shown two diffuse type of dielectric anomaly fo…
Three charge-ordering lanthanum nickelates La2-xAxNiO4, substituted with specific amounts of A = Sr, Ca, and Ba to achieve commensurate charge order, are investigated using broadband dielectric spectroscopy up to GHz frequencies. The transition temperatures of the samples are characterized by additional specific heat and magnetic susceptibility measurements. We find colossal magnitudes of the dielectric constant for all three compounds and strong relaxation features, which partly are of Maxwell-Wagner type arising from electrode polarization. Quite unexpectedly, the temperature-dependent colos…
We report on the synthesis of complex lead-free perovskite-type (1-x)(Ba$_{0.8}$Ca$_{0.2}$)TiO$_3$-xBi(Mg$_{0.75}$W$_{0.25}$)O$_3$ (BCT-xBMW) and (1-x)(Ba$_{0.8}$Ca$_{0.2}$)TiO$_3$-xBi(Mg$_{0.75}$Mo$_{0.25}$)O$_3$ (BCT-xBMM) solid solutions via conventional solid-state reaction route. The sintering temperature was adjusted as a function of composition x to obtain dense samples (relative densities over 95%) at the same time minimizing bismuth evaporation. X-ray diffraction analysis shows formation of single-phase perovskites for $0 \le x \le 0.10$ in the BCT-xBMW series and increasing concentra…
We report the dielectric properties of improper ferroelectric h-ErMnO$_3$. From the bulk characterisation we observe a temperature and frequency range with two distinct relaxation-like features, leading to high and even 'colossal' values for the dielectric permittivity. One feature trivially originates from the formation of a Schottky barrier at the electrode-sample interface, whereas the second one relates to an internal barrier layer capacitance (BLC). The calculated volume fraction of the internal BLC (of 8 %) is in good agreement with the observed volume fraction of insulating domain walls…
History-dependent and frequency-dependent dielectric nonlinearities induced by polar nanoregions in a thin film of 0.5 ( Ba 0.7 Ca 0.3 TiO 3 ) -- 0.5 ( BaZr 0.2 Ti 0.8 O 3 )
We present electrical transport measurements of heterostructures comprised of BaTiO$_3$ and Ba$_{1-x}$Sr$_x$TiO$_3$ epitaxially grown on Ge. The Sr-alloying imparts compressive strain to the BaTiO$_3$, which enables the thermal expansion mismatch between BaTiO$_3$ and Ge to be overcome to achieve $c$-axis oriented growth. The conduction bands of BaTiO$_3$ and Ba$_{1-x}$Sr$_x$TiO$_3$ are nearly aligned with the conduction band of Ge, which facilitates electron transport. Electrical transport measurements through the dielectric stack exhibit rectifying behavior and hysteresis, where the latter i…
Substrate temperature dependent dielectric and ferroelectric properties of (100) oriented lead-free Na$_{0.4}$K$_{0.1}$Bi$_{0.5}$TiO$_3$ thin films grown by pulsed laser deposition
The solid solution $0.5Ba(Ti_{0.8}Zr_{0.2})O_3$-$0.5(Ba_{0.7}Ca_{0.3})TiO_3$ (BCZT) has become a promising member of the lead-free piezoelectric materials because of its exceptionally high piezoelectric properties. In this study, we focus on studying pressure-dependent Raman spectroscopy, powder x-ray diffraction and dielectric constant measurements on BCZT. The data show several structural transitions are present, where the system from ambient mixed phase (tetragonal, {\it {P4mm}}+ orthorhombic {\it {Amm2}}) transforms into single phase ({\it {P4mm}}) at 0.26 GPa, then converts into cubic pha…
Subcoercive-field dielectric response of $0.5(\text{Ba}_{0.7}\text{Ca}_{0.3}\text{TiO}_{3})-0.5(\text{BaZr}_{0.2}\text{Ti}_{0.8}\text{O}_{3})$ thin film: peculiar third harmonic signature of phase transitions and residual ferroelectricity
Metallic nanoparticles embedded in dielectrics permit enhanced capture of light at specific wavelengths through excitation of plasmons, i.e. the quanta of coherent and collective oscillations of large concentrations of nearly free electrons. In order to maximize the potential of such enhanced absorption in useful tasks, such as the generation of carriers in photocatalysts and semiconductors, it is important to be able to predict and design plasmonic nanocomposites with desired wavelength-dependent optical absorption. Recently, a mixing approach formulated by Garcia and co-workers [Phys. Rev. B…
In this study, we have delineated the preparation and influence of Fe doping on microstructural and optical properties of the pristine and Fe incorporated TiO$_2$ thin film with different Fe concentrations (0, 2, 4, 6, and 8 at.% ). The samples are prepared by easier and cost-saving way of spray pyrolysis technique (SPT) using Ti(OCH$_2$CH$_2$CH$_2$CH$_3$)$_4$ as a precursor of mother material. The effect of Fe in the microstructure and phase formation of TiO$_2$ thin films is investigated by XRD analysis. XRD investigation depicts that the pristine product corresponds to anatase phase of TiO$…
Electric Charge Transport and Dielectric Properties of the Barium Titanate Ceramics Obtained by Spark-Plasma Sintering with Different Carbon Content
Institute of Physics of the National Academy of Sciences of Ukraine（乌克兰国家科学院物理研究所）；Educational Scientific Institute of High Technologies, Taras Shevchenko National University of Kyiv（基辅塔拉斯舍甫琴科国立大学高等技术教育科学研究所）；Frantsevich Institute for Problems in Materials Science, National Academy of Sciences of Ukraine（乌克兰国家科学院弗兰采维奇材料科学问题研究所）；Department of Chemistry, Stockholm University（斯德哥尔摩大学化学系）；Department of Physical Materials Science and Heat Treatment, National Technical University of Ukraine “Igor Sikorsky Kyiv Polytechnic Institute”（乌克兰国立技术大学“伊戈尔·西科尔斯基基辅理工学院”物理材料科学与热处理系）
In the present work, the effect of different nanofiller (BaTiO3, CeO2, Er2O3 or TiO2) on blend solid polymer electrolyte comprising of PEO and PVC complexed with bulky LiPF6 have been explored. The XRD analysis confirms the polymer nanocomposite formation. FTIR provides evidence of interaction among the functional groups of the polymer with the ions and the nanofiller in terms of shifting and changing peak profile. The highest ionic conductivity is ~2.3x10-5 S cm-1 with a wide electrochemical stability window of ~3.5 V for 10 wt. % Er2O3. The real and imaginary part of dielectric permittivity …
Quasiparticle excitation energies and optical properties of TiO$_{2}$ in the rutile and anatase structures are calculated using many-body perturbation theory methods. Calculations are performed for a frozen crystal lattice; electron-phonon coupling is not explicitly considered. In the GW method, several approximations are compared and it is found that inclusion of the full frequency dependence as well as explicit treatment of the Ti semicore states are essential for accurate calculation of the quasiparticle energy band gap. The calculated quasiparticle energies are in good agreement with avail…
