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We investigate the high temperature thermoelectric properties of Heusler alloys Fe2-xMnxCrAl (0<x<1). Substitution of 12.5% Mn at Fe-site (x = 0.25) causes a significant increase in high temperature resistivity (r{ho}) and an enhancement in the Seebe ck coefficient (S), as compared to the parent alloy. However, as the concentration of Mn is increased above 0.25, a systematic decrement in the magnitude of both parameters is noted. These observations have been ascribed (from theoretical analysis) to a change in band gap and electronic structure of Fe2CrAl with Mn-substitution. Due to absence of mass fluctuations and lattice strain, no significant change in thermal conductivity is seen across this series of Heusler alloys. Additionally, S drastically changes its magnitude along with a crossover from negative to positive above 900 K, which has been ascribed to the dominance of holes over electrons in high temperature regime. In this series of alloys, S and r{ho} shows a strong dependence on the carrier concentration and strength of d-d hybridization between Fe/Mn and Cr atoms.
We report the results of our investigation of the physical properties of mixed metal oxides RFe0.5Cr0.5O3 (R = Er and Yb). ErFe0.5Cr0.5O3 undergoes an antiferromagnetic ordering around 270 K followed by spin reorientation (SR) transitions around 150 and 8 K respectively. In contrast, in YbFe0.5Cr0.5O3 a single SR transition is noted at 36 K, below the AFM ordering temperature of 280 K. In ErFe0.5Cr0.5O3, a significant value of magnetic entropy change ({Delta}SM) ~ -12.4 J/kg-K is noted near the 2nd SR transition, however, this value is suppressed in YbFe0.5Cr0.5O3. Temperature dependent dielectric permittivity of ErFe0.5Cr0.5O3 and YbFe0.5Cr0.5O3 at different frequencies, reveal the presence of Debye-like relaxation behaviour in both compounds, which can be due to the effect of charge carrier hopping between localized states of Fe and Cr ions. Temperature dependent Raman scattering studies divulge that spin-phonon coupling plays a crucial role in defining the physical properties of these compounds.
We report structural, magnetic and dielectric properties of layered perovskite materials LnBaCuFeO5 (Ln = La and Lu). LaBaCuFeO5 shows magnetic cluster glass behavior below 60 K owing to the competing ferromagnetic and antiferromagnetic exchange inte ractions. Glassy dynamics of electric dipoles has also been observed in the vicinity of the magnetic glass transition temperature. The presence of significant coupling between spin and polar degrees of freedom results in the multiglass feature in LaBaCuFeO5. The LuBaCuFeO5 compound undergoes YBaCuFeO5 like commensurate to incommensurate antiferromagnetic transition at 175 K. Large magnetic irreversibility below 17 K in this compound suggests the presence of strong spin anisotropy. In addition, in this compound the interaction between the dipoles is not strong enough, which results in the absence of glassy dynamics of electric dipoles. The contrasting behavior of two compounds is possibly due to variation in the ferromagnetic and antiferromagnetic interactions along c-axis, which is the manifestation of structural modification arising out of the difference in the ionic radii of La and Lu.
We report a systematic investigation of the magnetic and magnetocaloric properties of Dy5Pd2 and Dy5PdNi. Our study on these compounds gave evidence that they exhibit complex magnetic behaviour along with the presence of glass-like magnetic phase. Fu rthermore, in these compounds both second order and first order phase transitions were present, which were validated through Arrott plots and Landau parameter analysis. AC susceptibility along with time dependent magnetisation study has confirmed the presence of double cluster glass-like freezing in both Dy5Pd2 and Dy5PdNi. These compounds show significant value of isothermal entropy change and relative cooling power and these values increased with Ni substitution. Beside conventional magnetocaloric effect, inverse magnetocaloric effect was noted in these compounds, which might arise due to the presence of complex non-equilibrium magnetic state. Along with these compounds a universal characteristic curve involving two other members of R5Pd2 family i.e. Er5Pd2 and Tb5Pd2 was constructed. The master curve reaffirmed the presence of both second and first order magnetic phase transition in such compounds which were in analogy to our results of Arrott plots and Landau parameter analysis. Additionally, magnetic entropy change followed the power law and the obtained exponent values indicated the presence of mixed magnetic interactions in these compounds.
We report the evolution of structural, magnetic and dielectric properties due to partial substitution of Ba by Sr in the high temperature multiferroic YBaCuFeO5. This compound exhibits ferroelectric and antiferromagnetic transitions around 200 K and these two phenomena are presumed to be coupled with each other. Our studies on magnetic and dielectric properties of the YBa1-xSrxCuFeO5 (x = 0.0, 0.25 and 0.5) show that substitution of Sr shifts magnetic transition towards higher temperature whereas dielectric transition to lower temperature. These results points to the fact that magnetic and dielectric transitions get decoupled as a result of chemical pressure in form of Sr substitution. The nature of magnetodielectric coupling changes across the series with the presence of higher order coupling terms. Additionally in these compounds glassy dynamics of electric dipoles is observed at low temperatures.
The polycrystalline form of the compound, Tb5Si3, crystallizing in Mn5Si3-type hexagonal structure, which was earlier believe to order antiferromagnetically below 69 K, has been recently reported by us to exhibit interesting magnetoresistance (MR) an omalies. In order to understand the magnetic anomalies of this compound better, we synthesized single crystals of this compound and subjected them to intense magnetization and MR studies. The results reveal that the magnetic behavior is strongly anisotropic as the easy axis is along a basal plane. There appear to be multiple magnetic features in the close vicinity of 70 K. In addition, there are multiple steps in isothermal magnetization (which could not be resolved in the data for polycrystalline data) for magnetic-field (H) along a basal plane. The sign of MR is positive in the magnetically ordered state, and, interestingly, the magnitude dramatically increases at the initial step for H parallel to basal plane, but decreases at subsequent steps as though the origin of these steps are different. However, for the perpendicular orientation (H || [0 0 0 1]), there is no evidence for any step either in M(H) or in MR(H). These results establish this compound is an interesting magnetic material.
We have investigated the magnetic behavior of ball-milled fine particles of well-known Kondo lattices, CeAu2Si2, CePd2Si2 and CeAl2, by magnetization and heat-capacity studies in order to understand the magnetic behavior when the particle size is red uced. These compounds have been known to order antiferromagnetically in the bulk form near (TN=) 10, 10 and 3.8 K respectively. We find that the features due to magnetic ordering get suppressed to temperatures below 1.8 K in the case of fine particles of ternary alloys, though trivalence of Ce as inferred from the effective moment remains unchanged. In contrast to this, in CeAl2, there appears to be a marginal enhancement of TN, when the particle size is reduced to less than a micron. These results can be consistently understood by proposing that there is relatively more 4f-localization as the particle size is reduced, resulting in weakening of exchange interaction strength.
The magnetic entropy change (DeltaS), a measure of the magnetocaloric effect, in Tb5Si3, a compound exhibiting unusual positive magnetoresistance following a magnetic-field-induced transition below magnetic transition temperature (~ 69 K), has been i nvestigated. We found that DeltaS is negative in the paramagnetic state. At the magnetic transition temperature, DeltaS shows sign reversal from negative (in the paramagnetic state) to positive value in the magnetically ordered state. The high-field state which is interestingly the high resistive state is found to be associated with higher entropy i.e. large positive DeltaS, behaving like a paramagnet. On the basis of this observation, we conclude that the magnetic field induces magnetic fluctuations in the system resulting in positive magnetoresistance, thereby rendering support to the idea of inverse metamagnetism in this compound. In addition, we note that Arrott plots present an interesting scenario.
Recently, we reported an anomalous enhancement of the positive magnetoresistance beyond a critical magnetic field in Tb5Si3 in the magnetically ordered state, attributable to inverse metamagnetism. This results in unusual magnetic hysteresis loops fo r the pressurized specimens, which are relevant to the topic of electronic phase separation. In this paper, we report the influence of small substitutions of Lu for Tb, to show the evolution of these magnetic anomalies. We find that, at low temperatures, the high-field high-resistivity phase could be partially stabilized on returning the magnetic field to zero in many of these Lu substituted alloys, as measured through the electrical resistivity ({rho}). Also, the relative fractions of this phase and the virgin phase appear to be controlled by a small tuning of the composition and temperature. Interestingly, at 1.8 K a sudden switch-over of the value of {rho} for this mixed phase to that for the virgin phase for some compositions is observed at low fields after a few field cycles, indicating metastability of this mixed phase.
The magnetic behavior of the quaternary compounds, RCr2Si2C (R = La, Ce), has been investigated by magnetization (M) and heat-capacity (C) measurements (1.8-300 K) in the bulk polycrystals and nano forms (<1 {mu}m) obtained by high-energy balling. Ou r finding is that Cr appears to exhibit magnetic ordering of an itinerant type at low temperatures (<20 K) in the bulk form, as inferred from a combined look at all the data. The magnetic ordering gets gradually suppressed with increasing milling time. Evidence for a mixed-valence state of Ce for the bulk form is obtained from the tendency of magnetic susceptibility to exhibit a maximum above 300 K. However, this feature vanishes in the nano form, which exhibits a Curie-Weiss behavior above 200 K as though Ce tends towards trivalency in these fine particles; in addition, there is a weak upturn in C/T below 10 K in the bulk, which becomes very prominent in the milled Ce-based specimens at lower temperatures, as though heavy-fermion behavior gets stronger in smaller particles.
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