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Register a new userQuantum Critical Points in Ferroelectric Relaxors: Stuffed Tungsten Bronze K3Li2Ta5O15 and Lead Pyrochlore (Pb2Nb2O7)
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We have synthesised ceramic specimens of the tetragonal tungsten bronze K3Li2Ta5O15 (KLT) and characterized its phase transition via X-ray, dielectric permittivity, ultrasonic spectroscopy and heat capacity measurements. The space group of KLT is reported as both P4/mbm or Cmmm with the orthorhombic distortion occurring when there are higher partial pressures of volatile K and Li used within the closed crucibles for the solid state synthesis. The data show strong relaxor behaviour, with the temperature at which the two dielectric relative permittivity peaks decreasing with 104 K $geqslant$ Tm1 $geqslant$ 69 K and 69 K $geqslant$ Tm2 $geqslant$ 46 K as probe frequency f is reduced from 1 MHz to 316 Hz. The data satisfy a Vogel-Fulcher model with an extrapolated freezing temperature for {epsilon} and {epsilon} of Tf1 = + 15.8 and - 11.8 K and Tf2 = - 5.0 and - 15.0 K for f $rightarrow$ 0 (tending to dc). Therefore by tuning frequency, the transition could be shifted to absolute zero suggesting KLT has a relaxor-type quantum critical point. In addition, we have reanalysed the conflicting literature for Pb2Nb2O7 pyrochlore which suggests that this is also a relaxor-type quantum critical point as the freezing temperature from Vogel-Fulcher fitting is below absolute zero. Since the transition temperature evidenced in the dielectric data at ca. 100 kHz shifts below zero Kelvin for very low frequencies, heat capacity data collected in the zero-frequency (dc) limit, should not indicate a transition. Both of these materials show promise as possible new relaxor-type quantum critical points within non-perovskite based structures as multiple compounds are reported with low-temperature transitions.
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Several Niobium oxides of formula Ba2LnFeNb4O15 (Ln = La, Pr, Nd, Sm, Eu, Gd) with the Tetragonal Tungsten Bronze (TTB) structure have been synthesised by conventional solid-state methods. The Neodymium, Samarium and Europium compounds are ferroelectric with Curie temperature ranging from 320 to 440K. The Praseodymium and Gadolinium compounds behave as relaxors below 170 and 300 K respectively. The Praseodymium, Neodymium, Samarium, Europium and Gadolinium compounds exhibit magnetic hysteresis loops at room temperature originating from traces of a barium ferrite secondary phase. The presence of both ferroelectric and magnetic hysteresis loops at room temperature allows considering these materials as composites multiferroic. Based on crystal-chemical analysis we propose some relationships between the introduction of Ln3+ ions in the TTB framework and the chemical, structural and physical properties of these materials.
Ferroelectric relaxors are complex materials with distinct properties. The understanding of their dielectric susceptibility, which strongly depends on both temperature and probing frequency, have interested researchers for many years. Here we report a macroscopic and phenomenological approach based on statistical modeling to investigate and better understand how the dielectric response of a relaxor depends on temperature. Employing the Maxwell-Boltzmann distribution and considering temperature dependent dipolar orientational polarizability, we propose a minimum statistical model and specific equations to understand and fit numerical and experimental dielectric responses versus temperature. We show that the proposed formula can successfully fit the dielectric response of typical relaxors, including Ba(Zr,Ti)O$_{3}$, Pb(Zn$_{1/3}$Nb$_{2/3}$)$_{0.87}$Ti$_{0.13}$O$_{3}$, and Pb(Mg$_{1/3}$Nb$_{2/3}$)O$_{3}$-0.05Pb(Zr$_{0.53}$Ti$_{0.47}$)O$_{3}$, which demonstrates the general applicability of this approach.
Materials with formula of A2B2O7 is a famous family with more than 300 compounds, and have abundant properties, like ferroelectric, multiferroic, and photocatalyst properties, etc. Generally, two structures dominate this family, which are pyrochlore and perovskite-like layered (PL) structure. Previously, the structure and properties design of these materials are usually complex, and solid solutions, which complicates the manufacture, as well as introducing complexity in the study of the microscopic origins of the properties. Here, we report that the pyrochlore-PL structure change happened in pure Eu2Ti2O7 under high pressure and temperature, and the formed PL structure will transfer back by heating. These results reveal that the PL structure formed in PL-pyrochlore solid solutions, is due to tuning of the high-pressure formed PL structure in pure pyrochlore compounds to ambient pressure. These results indicate the high pressure and high temperature can be used to manipulate the crystal structures from pyrochlore to PL structure, or vice versa. Furthermore, the PL Eu2Ti2O7 was confirmed as a lead free ferroelectric material for the first time.
The dielectric and magnetic polarizations of quantum paraelectrics and paramagnetic materials have in many cases been found to initially increase with increasing thermal disorder and hence exhibit peaks as a function of temperature. A quantitative description of these examples of order-by-disorder phenomenona has remained elusive in nearly ferromagnetic metals and in dielectrics on the border of displacive ferroelectric transitions. Here we present an experimental study of the evolution of the dielectric susceptibility peak as a function of pressure in the nearly ferroelectric material, strontium titanate, which reveals that the peak position collapses towards absolute zero as the ferroelectric quantum critical point is approached. We show that this behaviour can be described in detail without the use of adjustable parameters in terms of the Larkin-Khmelnitskii-Shneerson-Rechester (LKSR) theory, first introduced nearly 50 years ago, of the hybridization of polar and acoustic modes in quantum paraelectrics, in contrast to alternative models that have been proposed. Our study allows us to construct for the first time a detailed temperature-pressure phase diagram of a material on the border of a ferroelectric quantum critical point comprising ferroelectric, quantum critical paraelectric and hybridized polar-acoustic regimes. Furthermore, at the lowest temperatures, below the susceptibility maximum, we observe a new regime characterized by a linear temperature dependence of the inverse susceptibility that differs sharply from the quartic temperature dependence predicted by the LKSR theory. We find that this non-LKSR low temperature regime cannot be accounted for in terms of any detailed model reported in the literature, and its interpretation poses a new empirical and conceptual challenge.
Previous studies of Barkhausen noise in PZT have been limited to the energy spectrum (slew rate response voltages versus time), showing agreement with avalanche models; in barium titanate other exponents have been measured acoustically, but only at ambient temperatures. In the present study we report the Omori exponent (-0.95$pm$0.03) for aftershocks in PZT and extend the barium titanate studies to a wider range of temperature.
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