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Register a new userRelaxor ferroelectric behavior and intrinsic magnetodielectric behavior near room temperature in Li2Ni2Mo3O12, a compound with distorted honeycomb and spin-chains
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E. V. Sampathkumaran Professor
Publication date
2017
fields
Physics
and research's language is
English
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Keeping current interests to identify materials with intrinsic magnetodielectric behavior near room temperature and with novel pyroelectric current anomalies, we report temperature and magnetic-field dependent behavior of complex dielectric permittivity and pyroelectric current for an oxide, Li2Ni2Mo3O12, containing magnetic ions with (distorted) honey-comb and chain arrangement and ordering magnetically below 8 K. The dielectric data reveal the existence of relaxor ferroelectricity behavior in the range 160-240 K and there are corresponding Raman mode anomalies as well in that temperature range. Pyrocurrent behavior is also consistent with this interpretation, with the pyrocurrent peak-temperature interestingly correlating with the poling temperature. 7Li NMR offer an evidence for crystallographic disorder intrinsic to this compound and we therefore conclude that such a disorder is apparently responsible for the randomness of local electric field leading to relaxor ferroelectric property. Another observation of emphasis is that there is a notable decrease in the dielectric constant with the application of magnetic field to the tune of about -2.4% at 300 K, with the magnitude varying mariginally with temperature. Small loss factor values validate intrinsic behavior of the magnetodielectric effect at room temperature.
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We study themagnetism of a spin-1 substance Li2Ni2Mo3O12. The spin system consists of distorted honeycomb lattices and linear chains of Ni2+ spins. Li+ ions enter about 25% and 50% of the honeycomb and chain Ni sites, respectively, creating disorder in both spin subsystems. A magnetic phase transition occurs at Tc = 8.0 K in the zero magnetic field. In low magnetic fields, the magnetization increases rapidly below Tc, decreases below 7 K, and finally becomes negative at low temperatures. We determine the magnetic structure using neutron powder diffraction results. The honeycomb lattices and linear chains show antiferromagnetic and ferromagnetic long-range order, respectively. We investigate static and dynamic magnetic properties using the local probe technique of muon spin relaxation. We discuss the origin of the negative magnetization.
We present an extension and revision of the spectroscopic and structural data of the mixed stack charge transfer (CT) crystal 3,3$^prime$,5,5$^prime$-tetramethylbenzidine--tetrafluoro-tetracyanoquinodimethane (TMB-TCNQF$_4$), associated with new electric and dielectric measurements. Refinement of syncrotron structural data at low temperature have led to revise the previously reported [Phys. Rev. Mat. textbf{2}, 024602 (2018)] $C2/m$ structure. The revised structure is $P2_1/m$, with two dimerized stacks per unit cell, and is consistent with the vibrational data. However, polarized Raman data in the low-frequency region also indicate that by increasing temperature above 200 K the structure presents an increasing degree of disorder mainly along the stack axis. This finds confirmation in the analysis of the anisotropic displacement parameters of the structure. TMB-TCNQF$_4$ is confirmed to be a narrow gap semiconductor ($E_a sim 0.3$ eV) with room $T$ conductivity of $sim 10^{-4}~ Omega^{-1}$ cm$^{-1}$, while dielectric measurement have evidenced a typical relaxor ferroelectric behavior already at room $T$, with a peak in real part of dielectric constant $epsilon(T, u)$ around 200 K and 0.1 Hz. The relaxor behavior is explained in terms of the presence of spin solitons separating domains of opposite polarity that yield to ferrolectric nanodomains.
The magnetic behavior of the compound, Gd3Ru4Al12, which has been reported to crystallize in a hexagonal structure about two decades ago, had not been investigated in the past literature despite interesting structural features (that is, magnetic layers and triangles as well as Kagome-lattice features favouring frustrated magnetism) characterizing this compound. We report here the results of magnetization, heat-capacity, and magnetoresistance studies in the temperature (T) range 1.8-300 K. The results establish that there is a long-range magnetic order of an antiferromagnetic type below (TN= ) 18.5 K, despite a much large value (about 80 K) of paramagnetic Curie temperature with a positive sign characteristic of ferromagnetic interaction. We attribute this to geometric frustration. The most interesting finding is that there is an additional magnetic anomaly below about 55 K before the onset of long range order in the magnetic susceptibility data. Concurrent with this observation, the sign of isothermal entropy change remains positive above TN with a broad peak above TN. This observation indicates the presence of ferromagnetic clusters before the onset of long range magnetic order. Thus, this compound may serve as an example for a situation in which magnetic frustration due to geometrical reasons is faced by competition with such precursor effects. There is also a reversal of the sign of entropy-change in the curves for lower final fields (for H less than 30 kOe) on entering into magnetically ordered state consistent with the entrance into antiferromagnetic state. The magnetoresistance behavior is consistent with above conclusions.
The van der Waals ferromagnet Fe5GeTe2 has a Curie temperature TC of about 270 K, which can be raised above room temperature by tuning the Fe deficiency content. To achieve insights into its ferromagnetic exchange, we have studied the critical behavior by measuring the magnetization in bulk Fe5GeTe2 crystal around the ferromagnetic to paramagnetic phase transition. The analysis of the magnetization by employing various techniques including the modified Arrott plot, Kouvel-Fisher plot and critical isotherm analysis achieved a set of reliable critical exponents with TC = 273.7 K, beta = 0.3457, gamma = 1.40617, and delta = 5.021, suggesting a three-dimensional magnetic exchange with the distance decaying as J(r) ~ (r)$^-4.916, which is close to that of a three-dimensional Heisenberg model with long-range magnetic coupling.
We have recently reported that the Haldane spin-chain system, Er2BaNiO5, undergoing antiferromagnetic order below 32 K, is characterized by the onset of ferroelectricity near 60K due to magnetoelectric coupling induced by short-range magnetic-order within spin-chains. We have carried out additional magnetic and dielectric studies to understand the properties well below antiferromagnetic ordering temperature. We emphasize here on the following: (i) A strong frequency dependent behaviors of ac magnetic susceptibility and complex dielectric properties have been observed at much lower temperatures (below 8 K), that is, reentrant multiglass-like phenomenon, naturally suggesting the existence of an additional transition well below Neel temperature; ii) Magnetoelectric phase coexistence is observed at very low temperature (e.g., T =2K), where the high-field magnetoelectric phase is partially arrested on returning to zero magnetic field after a cycling through metamagnetic transition.
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