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Register a new userHysteretic Magnetic-Transport-Structural Transition in 114 Cobaltites: Size Mismatch Effect
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The triple magnetic-transport-structural transition versus temperature in three series of 114 cobaltites - Y1-xYbxBaCo4O7, Y1-xCaxBaCo4O7 and Yb1-xCaxBaCo4O7 - has been studied using magnetic, transport and differential scanning calorimetric measurements. The effect of the size mismatch {sigma}2, due to cationic disordering at the Ln sites upon such a transition is shown for the first time in a triangular lattice. We show that increasing <rLn> has an effect of increasing TS dramatically, while the size mismatch {sigma}2 at the Ln sites decreases TS substantially. Moreover, the cationic mismatch at the Ln sites modifies the nature of the hysteretic transition by turning the sharp first order transition seen in the undoped samples into an intermix of first and second order transitions. These results are discussed on the basis of the particular nature of the high temperature form which exhibits a hexagonal close packed structure (space group: P63mc) with respect to the low temperature orthorhombic form (space group: Pbn21), the latter corresponding to a distortion of the former due to a puckering of the kagome layers.
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Rare earth perovskite cobaltites are increasingly recognized as materials of importance due to rich physics and chemistry in their ordered-disordered structure for the same composition. Apart from colossal magnetoresistance effect, like manganites, the different forms of cobaltites exhibit interesting phenomena including spin, charge and orbital ordering, electronic phase separation, insulator-metal transition, large thermoelectric power at low temperature. Moreover, the cobaltites which display colossal magnetoresistance effect could be used as read heads in magnetic data storage and also in other applications depending upon their particular properties. The A-site ordereddisordered cobaltites exhibit ferromagnetism and metal-insulator transitions as well as other properties depending on the composition, size of A-site cations and various external factors such as pressure, temperature, magnetic field etc. Ordered cobaltites, having a 112-type layered structure, are also reported to have an effectively stronger electron coupling due to layered A-site cationic ordering. Most importantly for the present article we focus on La-Ba-Co-O based ordered-disordered perovskite phases, which exhibit interesting magnetic and electron transport properties with ferromagnetic transition, TC ~ 177K, and it being the first member of lanthanide series. Zener double exchange mechanism considered to be crucial for understanding basic physics of the ferromagneticmetallic phase, yet does not explain clearly the insulating-type phase. In terms of electron transport the ferromagnetic-metallic or insulating/semiconducting states have been discussed in the present article with different types of hopping model.
We present an extensive investigation (magnetic, electric and thermal measurements and X-ray absorption spectroscopy) of the Pr0.5Ca0.5CoO3 and (Pr1-yYy)0.7Ca0.3CoO3 (y=0.0625-0.15) perovskites, in which a peculiar metal-insulator (M-I) transition, accompanied with pronounced structural and magnetic anomalies, occurs at 76 K and 40-132 K, respectively. The inspection of the M-I transition using the XANES data of Pr L3-edge and Co K-edge proofs the presence of Pr4+ ions at low temperatures and indicates simultaneously the intermediate spin to low spin crossover of Co species on lowering the temperature. The study thus definitively confirms the synchronicity of the electron transfer between Pr3+ ions and Co^(3+/4+)O3 subsystem and the transition to the low-spin, less electrically conducting phase. The large extent of the transfer is evidenced by the good quantitative agreement of the determined amount of the Pr4+ species, obtained either from the temperature dependence of the XANES spectra or via integration of the magnetic entropy change over the Pr4+ related Schottky peak in the low-temperature specific heat. These results show that the average valence of Pr3+/Pr4+ ions increases (in concomitance with the decrease of the formal Co valence) below TMI for (Pr0.925Y0.075)0.7Ca0.3CoO3 up to 3.16+ (the doping level of the CoO3 subsystem decreases from 3.30+ to 3.20+), for (Pr0.85Y0.15)0.7Ca0.3CoO3 up to 3.28+ (the decrease of doping level from 3.30+ to 3.13+) and for Pr0.5Ca0.5CoO3 up to 3.46+ (the decrease of doping level from 3.50+ to 3.27+).
Hysteresis underlies a large number of phase transitions in solids, giving rise to exotic metastable states that are otherwise inaccessible. Here, we report an unconventional hysteretic transition in a quasi-2D material, EuTe4. By combining transport, photoemission, diffraction, and x-ray absorption measurements, we observed that the hysteresis loop has a temperature width of more than 400 K, setting a record among crystalline solids. The transition has an origin distinct from known mechanisms, lying entirely within the incommensurate charge-density-wave (CDW) phase of EuTe4 with no change in the CDW modulation periodicity. We interpret the hysteresis as an unusual switching of the relative CDW phases in different layers, a phenomenon unique to quasi-2D compounds that is not present in either purely 2D or strongly-coupled 3D systems. Our findings challenge the established theories on metastable states in density wave systems, pushing the boundary of understanding hysteretic transitions in a broken-symmetry state.
The d.c. magnetization and magnetic relaxation studies of the calcium doped samples, Y0.95Ca0.05BaCo2O5.5 and YBa0.95Ca0.05Co2O5.5, show the existence of a magnetic glass like behaviour in the family of cobaltites for the first time. Our investigations reveal glass-like arrest of kinetics at low temperature which prevents the system from reaching its magnetic ground state. We show that the low temperature state of these calcium doped phases, which consists of coexisting antiferromagnetic and ferro (or ferri) magnetic phase fractions, can be tuned in a number of ways. Our observations establish that the low temperature state of this oxide is not in thermal equilibrium. The glassy state is formed with the assistance of an external magnetic field, which makes it distinctly different from the more well known metastable state, the spin glass state. The cooling field can tune the fractions of the coexisting phases, and the glass-like state formed at low temperature can also be devitrified by warming the sample. The role of Ca doping in the appearance of these phenomena is discussed in terms of phase separation, involving Co3+ disproportionation into Co4+ ferromagnetic clusters and Co2+ antiferromagnetic clusters.
Here we report the evolution of structural, magnetic and transport properties in MnBi$_{2-x}$Sb$_x$Te$_4$ (0$leq x leq$2) single crystals. MnSb$_2$Te$_4$, isostructural to MnBi$_2$Te$_4$, has the lattice parameters of textit{a}=4.2445(3)$AA$ and textit{c}=40.869(5)$AA$, respectively. With increasing Sb content in MnBi$_{2-x}$Sb$_x$Te$_4$, the textit{a}-lattice decreases linearly following the Vegards law while the textit{c}-lattice shows little compositional dependence. The textit{a}-lattice contraction occurs by reducing Mn-Te-Mn bond angle while Mn-Te bond length remains nearly constant. The anisotropic magnetic properties suggest an antiferromagnetic order below T$_N$=19,K for MnSb$_2$Te$_4$ with the magnetic moments aligned along the crystallographic textit{c}-axis. The antiferromagnetic ordering temperature slightly decreases from 24,K for MnBi$_2$Te$_4$ to 19,K for MnSb$_2$Te$_4$. More dramatic change was observed for the critical magnetic fields required for the spin-flop transition and moment saturation. With increasing Sb content, both critical fields decrease and in MnSb$_2$Te$_4$ a small field of 3,kOe is enough to saturate the moment. In high magnetic fields, the saturation moment shows significant suppression from 3.56$mu_B$/Mn for MnBi$_2$Te$_4$ to 1.57$mu_B$/Mn for MnSb$_2$Te$_4$. Data analyses suggest that both the interlayer magnetic interaction and single ion anisotropy decrease with increasing Sb content. The partial substitution of Bi by Sb also dramatically affects the transport properties. A crossover from n-type to p-type conducting behavior is observed around x=0.63. Our results show close correlation between structural, magnetic and transport properties in MnBi$_{2-x}$Sb$_x$Te$_4$ and that partial substitution of Bi by Sb is an effective approach to fine tuning both the magnetism and transport properties of MnBi$_{2-x}$Sb$_x$Te$_4$.
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