Critical behavior and magnetocaloric effect across the magnetic transition in Mn1+xFe4-xSi3.

The nature of the magnetic transition, critical scaling of magnetization, and magnetocaloric effect in Mn1+xFe4-xSi3 (x = 0 to 1) are studied in detail. Our measurements show no thermal hysteresis across the magnetic transition for the parent compound which is in contrast with the previous report and corroborate the second order nature of the transition. The magnetic transition could be tuned continuously from 328 K to 212 K with Mn substitution at the Fe site. The Mn substitution leads to a linear increase in the unit cell volume and a slight reduction in the effective moment. A detailed critical analysis of the magnetization data for x = 0.0 and 0.2 is performed in the critical regime using the modified Arrott plots, Kouvel-Fisher plot, universal curve scaling, and scaling analysis of magnetocaloric effect. The magnetization isotherms follow modified Arrott plots with critical exponent (ß [Formula: see text] 0.308, γ [Formula: see text] 1.448, and δ [Formula: see text] 5.64) for the parent compound (x = 0.0) and (ß [Formula: see text] 0.304, γ [Formula: see text] 1.445, and δ [Formula: see text] 5.64) for x = 0.2. The Kouvel-Fisher and universal scaling plots of the magnetization isotherms further confirm the reliability of our critical analysis and values of the exponents. These values of the critical exponents are found to be same for both the parent and doped samples which do not fall under any of the standard universality classes. The exchange interaction decays as J(r) ~ r-3.41 following the renormalization group theory and the observed critical exponents correspond to lattice dimensionality d = 2, spin dimensionality n = 1, and the range of interaction σ = 1.41. This value of σ(<2) indicates long-range interaction between magnetic spins. A reasonable magnetocaloric effect ΔSm [Formula: see text] -6.67 J/Kg-K and -5.84 J/Kg-K for x = 0.0 and 0.2 compounds, respectively, with a huge relative cooling power (RCP ~ 700 J/Kg) for 9 T magnetic field change is observed. The universal scaling of magnetocaloric effect further mimics the second order character of the magnetic transition. The obtained critical exponents from the critical analysis of magnetocaloric effect agree with the values deduced from the magnetic isotherm analysis.

Note: Inverted heat pulse method to measure heat capacity during cooling: A counterpart of conventional quasi-adiabatic heat pulse method.

A simple method to extract known amount of heat from a sample within a given time interval has been proposed. Using this method, which we call inverted heat pulse (IHP) method, absolute values of heat capacity (C(P)) during cooling can be measured in a manner similar to conventional quasi-adiabatic heat pulse method of measuring C(P) during warming. Absolute accuracy of the measured C(P) using IHP method is found to be better than 2% in the temperature range 100-300 K. Applicability of this method to a broad and hysteretic first order transition is tested by measuring C(P) of Rh doped FePt sample, which shows a antiferromagnetic to ferromagnetic first order transition with a transition width of ∼35 K and hysteresis of ∼6 K. The peak value of the measured C(P) using IHP during cooling as well as entropy change calculated from measured data is found to be in good agreement with that measured during warming using conventional quasi-adiabatic heat pulse method.

Low temperature high magnetic field 57Fe Mössbauer study of kinetic arrest in Ta doped HfFe2.

Low temperature high magnetic field (57)Fe Mössbauer measurements were carried out on the inter-metallic compound Hf0.77Ta0.23Fe2 by following novel paths in H-T space. The ferromagnetic (FM) fraction at 5 K and zero magnetic field is shown to depend on the cooling field, i.e., the higher the field is, the higher the FM fraction is. Mössbauer spectra collected in the presence of a 4 T magnetic field show that the antiferromagnetic (AFM) spins are canted with respect to the applied magnetic field and hence contribute to the total bulk magnetization in this compound. The data also show an induced magnetic moment even at the 2a site of the AFM phase. Mössbauer spectra collected using the CHUF (cooling and heating in un-equal magnetic fields) protocol show a reentrant transition when the sample is cooled in zero field and measured during warming in 4 T, showing the FM state as the equilibrium state. This work is the first microscopic experimental evidence for the de-vitrification of the kinetically arrested magnetic state.

Concentration dependence in kinetic arrest of the first-order magnetic transition in Ta doped HfFe2.

Magnetic behavior of the pseudo-binary alloy Hf(1-x)Ta(x)Fe(2) has been studied, for which the zero-field ferromagnetic (FM) to antiferromagnetic (AFM) transition temperature is tuned near to T = 0 K. Our studies show that such composition lies around x = 0.230. Detailed magnetization studies on x = 0.225, 0.230 and 0.235 show thermomagnetic irreversibility at low temperature due to kinetic arrest of the first-order AFM-FM transition. All three compositions studied show a reentrant transition in the zero-field-cooled warming curve and non-monotonic variation of the upper critical field. The region in H-T space where these features of kinetic arrest manifest themselves increases with increasing Ta concentration.

The metal-insulator transition in nanocrystalline Pr0.67Ca0.33MnO3: the correlation between supercooling and kinetic arrest.

The transition and hysteresis widths of a disorder broadened first order magnetic transition vary in H-T space which influences the co-existing phase fraction at low temperature arising due to kinetic arrest of the first order transition. We explored the role of change in the relative width of the supercooling/superheating band and kinetic arrest band for a ferromagnetic metallic to antiferromagnetic insulating transition. It is shown that for a correlated kinetic arrest and supercooling bands, the topology of the devitrification curves (or transformation across the (H(K),T(K)) band during warming) changes with the change in the relative width of these two bands. In addition to this, for a broader kinetic arrest band, the transformation temperature across the superheating band under constant H now depends on the arrested phase fraction. These predictions have been tested on nanocrystalline Pr(0.67)Ca(0.33)MnO(3), which is known to show a large variation in hysteresis width in H-T space. This is the first report where correlation between the kinetic arrest band and the supercooling band has been shown experimentally, in contrast to the universal observation of anticorrelation reported so far.

First-order antiferro-ferromagnetic transition in Fe(49)(Rh(0.93)Pd(0.07))(51) under simultaneous application of magnetic field and external pressure.

A magnetic field-pressure-temperature (H-P-T) phase diagram for first-order antiferromagnetic (AFM) to ferromagnetic (FM) transitions in Fe(49)(Rh(0.93)Pd(0.07))(51) has been constructed using resistivity measurements under simultaneous application of magnetic field (up to 8 T) and pressure (up to 20 kbar). The temperature dependence of resistivity (ρ-T) shows that the width of the transition and the extent of hysteresis decreases with pressure and increases with magnetic field. By exploiting opposing trends of dT(N)/dP and dT(N)/dH (where T(N) is the first-order transition temperature), the relative effects of temperature, magnetic field and pressure on disorder-broadened first-order transitions has been studied. For this, a set of H and P values are chosen for which T(N)(H(1),P(1)) = T(N)(H(2),P(2)). Measurements for such combinations of H and P show that the temperature dependence of resistivity is similar, i.e. the broadening (in temperature) of transition as well as the extent of hysteresis remains independent of H and P. Isothermal magnetoresistance measurements under various constant pressures show that even though the critical field required for AFM-FM transition depends on applied pressure, the extent of hysteresis as well as transition width (in magnetic field) remains constant with varying pressure.