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Register a new userFerroelectricity in (Pb$_y$Sn$_{1-y}$)$_2$P$_2$S$_6$ mixed crystals and random field BEG model
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For Sn$_2$P$_2$S$_6$ ferroelectrics the second order phase transitions line is observed until reaching the tricritical point at transition temperature lowering to 250 K by compression. Observed temperature-pressure phase diagram agrees with simulated diagram by MC calculations based on early founded by DFT study local potential for Sn$_2$P$_2$S$_6$ crystals. In addition to the tricritical point, the possibility of disordered and quadrupolar phases occurrence was shown. For mixed crystals with tin by lead substitution, the investigated ultrasound, hypersound and low frequency dielectric properties also reveal appearance of heterophase peculiarities at decreasing of ferroelectric transition temperature below so named temperature waterline near 250~K. The tricriticality at similar temperature level also appears in mixed crystals at sulfur by selenium substitution. Such behavior agree with Blume-Emery-Griffiths (BEG) model, that is appropriated for investigated ferroelectric system with three-well local potential for the order parameter (spontaneous polarization) fluctuations.
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The valence fluctuations which are related to the charge disproportionation of phosphorous ions $P^{4+} + P^{4+}rightarrow P^{3+} + P^{5+}$ are the origin of ferroelectric and quantum paraelectric states in Sn(Pb)$_2$P$_2$S$_6$ semiconductors. They involve recharging of SnPS$_3$ or PbPS$_3$ structural groups which could be represented as half-filled sites in the crystal lattice. Temperature-pressure phase diagram for Sn$_2$P$_2$S$_6$ compound and temperature-composition phase diagram for (Pb$_y$Sn$_{1-y}$)$_2$P$_2$S$_6$ mixed crystals, which include tricritical points and where a temperature of phase transitions decrease to 0 K, together with the data about some softening of low energy optic phonons and rise of dielectric susceptibility at cooling in quantum paraelectric state of Pb$_2$P$_2$S$_6$, are analyzed by GGA electron and phonon calculations and compared with electronic correlations models. The anharmonic quantum oscillators model is developed for description of phase diagrams and temperature dependence of dielectric susceptibility.
The dipole ordering in Sn(Pb)$_2$P$_2$S(Se)$_6$ materials may be tuned by chemical substitution realizing a ferroelectric quantum phase transition and quantum glassy or relaxor type phenomena on different parts of the phase diagram. The introduction of Ge impurity increases the temperature of the phase transitions and initiates a more pronounced Ising type critical anomaly in Sn$_2$P$_2$S$_6$ crystal, does not shift the coordinate of the Lifshitz point $x_{textrm {LP}}$ in Sn$_2$P$_2$(Se$_x$S$_{1-x}$)$_6$ mixed crystals, induces the appearance of a ferroelectric phase transition in quantum paraelectrics Pb$_2$P$_2$S$_6$ and inhomogeneous polar ordering in (Pb$_{0.7}$Sn$_{0.3}$)$_2$P$_2$S(Se)$_6$ crystals. For Pb$_2$P$_2$S$_6$ crystal, the real part of the dielectric susceptibility in the quantum critical regime varies as $1/T^2$ instead of the expected $1/T^3$ behavior for uniaxial materials. This can be partially explained by a screening phenomenon in the semiconductor materials of the Sn(Pb)$_2$P$_2$S(Se)$_6$ system, which weakens the long range electric dipole interactions, and also provides, at high temperatures, a critical behavior near the Lifshitz point (studied by thermal diffusivity) similar to the one predicted in the case of systems with short range interactions. At low temperatures, a quantum critical behavior in Pb$_2$P$_2$S$_6$ crystal can be established by the nonlinear coupling between polar and antipolar fluctuations. An increase in thermal conductivity is induced by Ge impurity in Pb$_2$P$_2$S$_6$ crystal, which is explained through the weakening of the acoustic phonons resonance scattering by soft optic phonons because of the appearance of ferroelectric phase polar clusters.
Magnetoresistance (MR) of the Bi$_{2-x}$Pb$_x$Sr$_2$Co$_2$O$_y$ ($x$=0, 0.3, 0.4) single crystals is investigated systematically. A nonmonotonic variation of the isothermal in-plane and out-of-plane MR with the field is observed. The out-of-plane MR is positive in high temperatures and increases with decreasing $T$, and exhibits a pronounced hump, and changes the sign from positive to negative at a centain temperature. These results strongly suggest that the observed MR consists of two contributions: one emph{negative} and one emph{positive} component. The isothermal MR in high magnetic fields follows a $H^2$ law. While the negative contribution comes from spin scattering of carriers by localized-magnetic-moments based on the Khosla-Fischer model.
Layered multi-ferroic materials exhibit a variety of functional properties that can be tuned by varying the temperature and pressure. As-synthesized CuInP$_2$S$_6$ is a layered material that displays ferrielectric behavior at room temperature. When synthesized with Cu deficiencies, CuInP$_2$S$_6$ spontaneously phase segregates to form ferrielectric CuInP$_2$S$_6$ (CIPS) and paraelectric In$_{4/3}$P$_2$S$_6$ (IPS) domains in a two-dimensional self-assembled heterostructure. Here, we study the effect of hydrostatic pressure on the structure of Cu-deficient CuInP$_2$S$_6$ by Raman spectroscopy measurements up to 20 GPa. Detailed analysis of the frequencies, intensities, and linewidths of the Raman peaks reveals four discontinuities in the spectra around 2, 10, 13 and 17 GPa. At ~2 GPa, we observe a structural transition initiated by the diffusion of IPS domains, which culminates in a drastic reduction of the number of peaks around 10 GPa. We attribute this to a possible monoclinic-trigonal phase transition at 10 GPa. At higher pressures (~ 13 GPa), significant increases in peak intensities and sharpening of the Raman peaks suggest a bandgap-lowering and an isostructural electronic transition, with a possible onset of metallization at pressures above 17 GPa. When the pressure is released, the structure again phase-separates into two distinct chemical domains within the same single crystalline framework -- however, these domains are much smaller in size than the as-synthesized material resulting in suppression of ferroelectricity through nanoconfinement. Hydrostatic pressure can thus be used to tune the electronic and ferrielectric properties of Cu-deficient layered CuInP$_2$S$_6$.
We report an optimized chemical vapor transport method to grow single crystals of (Mn$_{1-x}$Ni$_x$)$_2$P$_2$S$_6$ where x = 0, 0.3, 0.5, 0.7 & 1. Single crystals up to 4,mm,$times$,3,mm,$times$,200,$mu$m were obtained by this method. As-grown crystals characterized by means of scanning electron microscopy, and powder x-ray diffraction measurements. The structural characterization shows that all crystals crystallize in monoclinic symmetry with the space group $C2/m$ (No. 12). We have further investigated the magnetic properties of this series of single crystals. The magnetic measurements of the all as-grown single crystals show long-range antiferromagnetic order along all crystallographic principal axes. Overall, the Neel temperature TN is non-monotonous, with increasing $Ni^{2+}$ doping the temperature of the antiferromagnetic phase transition first decreases from 80 K for pristine Mn$_2$P$_2$S$_6$ (x = 0) up to x = 0.5, and then increases again to 155 K for pure Ni$_2$P$_2$S$_6$ (x = 1). The magnetic anisotropy switches from out-of-plane to in-plane as a function of composition in (Mn$_{1-x}$Ni$_x$)$_2$P$_2$S$_6$ series. Transport studies under hydrostatic pressure on the parent compound Mn$_2$P$_2$S$_6$ evidence an insulator-metal transition at an applied critical pressure of ~22 GPa
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