Effect of Si substitution in ferromagnetic Pr2Fe17: a magnetocaloric material with zero thermal expansion operative at high temperature.

This article deals with the magnetic and thermal expansion properties of Pr2Fe16Si. This compound has been well characterized from the structural point of view by analysing X-ray diffraction (XRD) patterns. The temperature dependent behaviour of magnetization (M) and the structural parameters (lattice parameters, unit cell volume) suggest that the compound undergoes a second order phase transition from a paramagnetic to a ferromagnetic state at TC = 390 K, driven by an increase in bond length between iron atoms at 6c sites. The field-dependent behaviour of M below TC, and comparatively lower value of coercivity (Hc) have been explained by the role of Si atoms as pinning centres. In the ferromagnetic phase, the system is found to behave like an inhomogenous mean field system. The study of thermal expansion properties establishes that the compound is a zero thermal expansion material (αv = 5.3 × 10-6 K-1) operative in the temperature range T = 200-340 K. As a magnetocaloric material, Pr2Fe16Si possesses high RCP (87 J kg-1 at µ0H = 1.5 T), high operating temperature (390 K) and moderate |ΔSM|max.

Physical properties of RIr3 (R = Gd, Tb, Ho) compounds with coexisting polymorphic phases.

The binary compounds GdIr3, TbIr3 and HoIr3 are synthesized successfully and found to form with macroscopic co-existence of two polymorphic phases: AuBe5 (C15b) and AuCu3-type. The dc magnetization and heat capacity studies confirm that the C15b phase orders ferromagnetically, whereas the AuCu3 phase remains paramagnetic down to 2 K. The frequency dependent ac-susceptibility data, time dependent magnetic relaxation behavior and magnetic memory effect studies suggest that TbIr3 and HoIr3 are cannonical spin-glass systems, but no glassy feature could be found in GdIr3. The critical behavior of all three compounds has been investigated using the magnetization and heat capacity measurements around the transition temperature (TC). The critical exponents α, ß, γ and δ have been estimated using different techniques such as the Arrott-Noakes plot, Kouvel-Fisher plot and critical isotherm as well as analysis of specific heat data and study of magnetocaloric effect. The critical analysis study identifies the type of universal magnetic class in which the three compounds belong.

Transverse vibration driven large uniaxial negative and zero thermal expansion in boron bridged REPt3B framework materials.

In this work anomalous uniaxial thermal expansion behaviour at low temperatures along the c-direction of the tetragonal phase of different members of the antiperovskite REPt3B (RE = Sm, Gd-Tm) compounds is reported. Negative or zero thermal expansion (NTE/ZTE) behaviour in these compounds arises due to the transverse vibration of boron atoms in the linear Pt-B-Pt linkage. The coefficient of thermal expansion along the c-axis tends to become more negative in annealed compounds in comparison to those estimated for as-cast samples. While the as-cast TmPt3B and HoPt3B exhibit essentially ZTE behaviour, the NTE coefficient of annealed GdPt3B (∼-28 ppm K-1) is found to be even larger than that of the well known framework material ZrW2O8 (∼-9 ppm K-1) reported in the literature.

Observation of short range order driven large refrigerant capacity in chemically disordered single phase compound Dy2Ni0.87Si2.95.

In this work, we report the successful synthesis of a new intermetallic compound Dy2Ni0.87Si2.95 forming in single phase only with a chemically disordered structure. The random distribution of Ni/Si and crystal defects create a variation in the local electronic environment between the magnetic Dy ions. In the presence of both disorder and competing exchange interactions driven magnetic frustration, originating due to c/a ∼ 1, the compound undergoes spin freezing behaviour below 5.6 K. In the non-equilibrium state below the spin freezing behaviour, the compound exhibits aging phenomena and magnetic memory effects. In the magnetically short-range ordered region, much above the freezing temperature, an unusual occurrence of considerable magnetic entropy change, -ΔSmaxM ∼ 21 J kg-1 K-1 with large cooling power RCP ∼ 531 J kg-1 and adiabatic temperature change, ΔTad ∼ 10 K for a field change of 70 kOe, is observed for this short range ordered cluster-glass compound without any magnetic hysteresis loss.

Chemical disorder driven reentrant spin cluster glass state formation and associated magnetocaloric properties of Nd2Ni0.94Si2.94.

In this work, we report the synthesis of a new ternary intermetallic compound, Nd2Ni0.94Si2.94, that forms in single phase only in a defect crystal structure. The compound exhibits an antiferromagnetic transition below 7.2 K (TN) followed by a spin cluster freezing behaviour below 2.85 K (Tf), which makes the compound a reentrant spin cluster glass system. The detailed studies of dc and ac magnetization, heat capacity, non-equilibrium dynamical behaviour, viz., aging effect, temperature and field dependent magnetic relaxation and magnetic memory effect establish the compound to be a cluster-glass material below freezing temperature. The interplay between competing exchange coupling (c/a ≃ 1.04 ⇒ JNN ≃ JNNN) and chemical disorder driven variation in the electronic environment among the Nd ions has been argued to be responsible for such a metastable state formation. A considerable value of MCE parameters (-ΔS ∼ 11.4 J kg-1 K-1, RCP ∼ 160 J kg-1 and ΔTad ∼ 5.2 K for a field change of 70 kOe) is obtained for this magnetically frustrated glassy compound.

Structural Transformation in Inverse-Perovskite REPt3B (RE = Sm and Gd-Tm) Associated with Large Volume Reduction.

In this work, we report the structural phase transformation of tetragonal inverse-perovskite REPt3B (RE = Sm, and Gd-Tm) compounds to cubic perovskite structure, with a large volume reduction of about 9% (reduction of the c axis, ∼17%; increase in the a axis, ∼5%). The structural stability of the cubic phase, however, could only be maintained by lowering the lattice parameter of the off-stoichiometric REPt3Bx (x < 1), formed in the process of annealing. The combined effect of phase transformation and stoichiometric defects is argued to be responsible for the observed volume collapse. Unexpectedly, the application of a large hydrostatic pressure of ∼20 GPa does not have any significant effect on the crystal structure. Neutron diffraction studies and heat capacity measurements unambiguously confirm different magnetic transition temperatures in the tetragonal and cubic phases. The different physical properties of these two phases demonstrate the interrelationship between the crystal chemistry and the physics of the system. The synthetic route to cubic REPt3Bx identified in this work may be utilized to prepare new ternary rare-earth intermetallics in a cubic perovksite form, which was previously found to facilitate unconventional superconductivity.

Complex magnetic properties associated with competing local and itinerant magnetism in [Formula: see text].

Ternary intermetallic compound [Formula: see text] has been synthesized in single phase and characterized by x-ray diffraction, scanning electron microscopy with energy dispersive x-ray spectroscopy (SEM-EDX) analysis, magnetization, heat capacity, neutron diffraction and muon spin rotation/relaxation ([Formula: see text]SR) measurements. The polycrystalline compound was synthesized in single phase by introducing necessary vacancies in Co/Si sites. Magnetic, heat capacity, and zero-field neutron diffraction studies reveal that the system undergoes magnetic transition below [Formula: see text]4 K. Neutron diffraction measurement further reveals that the magnetic ordering is antiferromagnetic in nature with an weak ordered moment. The high temperature magnetic phase has been attributed to glassy in nature consisting of ferromagnetic clusters of itinerant (3d) Co moments as evident by the development of internal field in zero-field [Formula: see text]SR below 50 K. The density-functional theory (DFT) calculations suggest that the low temperature magnetic transition is associated with antiferromagnetic coupling between Pr 4f and Co 3d spins. Pr moments show spin fluctuation along with unconventional orbital moment quenching due to crystal field. The evolution of the symmetry and the crystalline electric field environment of Pr-ions are also studied and compared theoretically between the elemental Pr and when it is coupled with other elements such as Co. The localized moment of Pr 4f and itinerant moment of Co 3d compete with each other below [Formula: see text]20 K resulting in an unusual temperature dependence of magnetic coercivity in the system.

Studies on magnetocaloric effect of Tb2Ni0.90Si2.94 compound.

A comparative study has been carried out on the magnetocaloric properties of as-cast and annealed Tb2Ni0.90Si2.94 intermetallic compound. While the as-cast material exhibits ferromagnetic cluster-glass behaviour below 9.9 K coexisting with antiferromagnetic (AFM) interaction, the annealed system shows AFM ordering below 13.5 K and spin freezing occurs below 4 K. The compound exhibits moderate magnetocaloric performance with maximum isothermal entropy changes (-ΔS M) 8.8 and 10.9 J kg-1 K-1, relative cooling power (RCP) 306 and 365 J kg-1, along with adiabatic temperature change (ΔT ad) 5.5 and 8.15 K for 70 kOe magnetic field change in as-cast and annealed forms, respectively. The estimated magnetic entropy change is found to be larger for annealed sample in comparison to that of as-cast analogue. However, the full width at half maxima (FWHM) of -ΔS M(T) behaviour is larger in as-cast compound due to the presence of inherent structural disorder which reduces with thermal annealing. A positive isothermal entropy change (-ΔS M) and adiabatic temperature change (ΔT ad) is observed for the as-cast compound in the measured field and temperature region. In contrast, the annealed system exhibits inverse magnetocaloric effect in the low field and temperature region where AFM interactions dominate. Magnetocaloric effect (MCE) is used as a tool to establish a subtle correlation between the observed magnetocaloric effect and the reported magnetic properties of the system.

Negative pressure driven valence instability of Eu in cubic Eu(0.4)La(0.6)Pd(3).

We report the change in the valency of Eu-ions in the binary intermetallic cubic compound EuPd(3) induced by La doping at rare-earth sites. Doping of La generates negative chemical pressure in the lattice, resulting in a significant increase of the lattice parameter without altering the simple-cubic structure of the compound. Results of dc-magnetic measurements suggest that this increase in the lattice parameter is associated with the valence transition of Eu-ions from Eu(3+) to a mixed-valent state. As Eu(2+)-ions possess a large magnetic moment, this valence transition significantly modifies the magnetic behavior of the compound. In contrast to introducing boron at the vacant body center site of the unit cell to change the valency of Eu-ions, as in the case of EuPd(3)B, our results suggest it can also be altered by doping a rare-earth ion of larger size at the lattice site of Eu in EuPd(3).

Role of random magnetic anisotropy on the valence, magnetocaloric and resistivity properties in a hexagonal Sm2Ni0.87Si2.87 compound.

In this work, we report the effect of random magnetic anisotropy (RMA) on the valence, magnetocaloric and resistivity properties in a glassy intermetallic material Sm2Ni0.87Si2.87. On the basis of detailed studies on the valence band and core level electronic structure, we have established that both the Sm3+ and Sm2+ ions are present in the system, suggesting the compound to be of mixed valence in nature. The significant observation of positive magnetic entropy change in zero-field cooled measurement has been argued due to the presence of RMA that develops due to local electronic environmental variations between the rare-earth ions in the system. The quantum interference effect caused by the elastic electron-electron interaction is responsible for the resistivity upturn at low-temperature for this disordered metallic conductor.

Unusual bidirectional frequency dependence of dynamical susceptibility in hexagonal intermetallic Pr2Ni0.95Si2.95.

In this study, the synthesis of a novel ternary intermetallic compound Pr2Ni0.95Si2.95 forming in single phase only by deliberately introducing vacancies in Ni/Si site is reported. The detailed studies on dc magnetization, heat capacity, ac magnetization & associated dynamical scaling, different types of non-equilibrium dynamical behaviour, viz., magnetic relaxation behaviour as a function of wait time and temperature, aging phenomena, and magnetic memory effect firmly establish that the compound exhibits spin freezing behaviour below 3.3 K (Tf). However, below Tf, temperature dependence of ac susceptibility data exhibit an additional peak that shows reverse frequency dependence to that generally observed in a glassy system. The unusual bidirectional frequency dependence in a single magnetic system is of significant interest and rarely reported in literature. Competing exchange interaction arising from c/a ~ 1 and crystallographic randomness driven magnetic phase separation has been argued to be responsible for such observation. The reverse frequency shift of the low temperature peak has been described on the basis of a simple phenomenological model proposed in this work.

Low-field induced large magnetocaloric effect in Tm2Ni0.93Si2.93: influence of short-range magnetic correlation.

In this work, we report the successful synthesis of a new intermetallic compound Tm2 [Formula: see text] [Formula: see text] that forms in single phase only in defect crystal structure. The compound does not show any long range magnetic ordering down to 2 K. The material exhibits a large magnetic entropy change ([Formula: see text] J [Formula: see text] K-1) and adiabatic temperature change ([Formula: see text] K) at 2.2 K for a field change of 20 kOe which can be realized by permanent magnets, thus being very beneficial for application purpose. In the absence of long-range magnetic ordering down to 2 K, the metastable nature of low-temperature spin dynamics and short-range magnetic correlations are considered to be responsible for such a large magnetocaloric effect over a wide temperature region.

Magnetic frustration induced large magnetocaloric effect in the absence of long range magnetic order.

We have synthesized a new intermetallic compound Ho2Ni0.95Si2.95 in a single phase with a defect crystal structure. The magnetic ground state of this material found to be highly frustrated without any long range order or glassy feature as investigated through magnetic, heat capacity and neutron diffraction measurements. The interest in this material stems from the fact that despite the absence of true long range order, large magnetocaloric effect (isothermal magnetic entropy change, -ΔSM ~ 28.65 J/Kg K (~205.78 mJ/cm3 K), relative cooling power, RCP ~ 696 J/Kg (~5 J/cm3) and adiabatic temperature change, ΔT ad ~ 9.32 K for a field change of 70 kOe) has been observed which is rather hard to find in nature.

Multiple crossovers between positive and negative magnetoresistance versus field due to fragile spin structure in metallic GdPd3.

Studies on the phenomenon of magnetoresistance (MR) have produced intriguing and application-oriented outcomes for decades-colossal MR, giant MR and recently discovered extremely large MR of millions of percents in semimetals can be taken as examples. We report here the discovery of novel multiple sign changes versus applied magnetic field of the MR in the cubic intermetallic compound GdPd3. Our study shows that a very strong correlation between magnetic, electrical and magnetotransport properties is present in this compound. The magnetic structure in GdPd3 is highly fragile since applied magnetic fields of moderate strength significantly alter the spin arrangement within the system-a behavior that manifests itself in the oscillating MR. Intriguing magnetotransport characteristics of GdPd3 are appealing for field-sensitive device applications, especially if the MR oscillation could materialize at higher temperature by manipulating the magnetic interaction through perturbations caused by chemical substitutions.

Role of the stability of charge ordering in exchange bias effect in doped manganites.

In this work we have carried out an elaborate study on the magnetic properties and investigated the exchange bias phenomena of some charge-ordered (CO) manganites. The detailed study of Sm1-x Ca x MnO3 (x = 0.5, 0.55, 0.6, 0.65, 0.7) compounds shows that Sm0.4Ca0.6MnO3, which is the most robust charge ordered material studied here, shows significantly large exchange bias field (HE) as compared to the other compounds. Our experimental results and analysis indicate that TCO, which reflects the stability of the charge-ordered state, is one of the key parameters for the exchange bias effect. Similar behaviour is found in other rare-earth analogues, viz., La1-x Ca x MnO3 and Pr1-x Ca x MnO3 compounds as well. We also found that with increasing stability of CO states in Sm1-x Ca x MnO3 compounds, HE enhances due to increase in number and reduction in size of ferromagnetic clusters.

Griffiths phase behaviour in a frustrated antiferromagnetic intermetallic compound.

The rare coexistence of a Griffiths phase (GP) and a geometrically frustrated antiferromagnetism in the non-stoichiometric intermetallic compound GdFe0.17Sn2 (the paramagnetic Weiss temperature θp ~ -59 K) is reported in this work. The compound forms in the Cmcm space group with large structural anisotropy (b/c ~ 4). Interestingly, all the atoms in the unit cell possess the same point group symmetry (Wycoff position 4c), which is rather rare. The frustration parameter, f = |θp|/TN has been established as 3.6, with the Néel temperature TN and Griffiths temperature TG being 16.5 and 32 K, respectively. The TG has been determined from the heat capacity measurement and also from the magnetocaloric effect (MCE). It is also shown that substantial difference in GP region may exist between zero field and field cooled measurements - a fact hitherto not emphasized so far.

A distributed simulation technique for multiple input multiple output systems.

Distributed computing concepts have been attempted in the realm of real-time process control for a long time. This started with the systolic arrays of processors and an enormous amount of research has been done in this field. This paper proposes a methodology by which a multiple input multiple output system representing a plant and defined in terms of connected blocks of transfer functions can be decomposed into a set of parallel simulation processes in a message passing environment viz. a network of work stations. The paper also analyzes the scope of optimization of the processing time associated with each task. The methodology includes online reconfiguration of the system.