Pol Lloveras

Barocaloric and magnetocaloric effects in Fe49Rh51

We report on calorimetry under applied hydrostatic pressure and magnetic field at the antiferromagnetic-ferromagnetic (AFM/FM) transition of Fe49Rh51. Results demonstrate the existence of a giant barocaloric effect in this alloy, a functional property that adds to the magnetocaloric and elastocaloric effects previously reported for this alloy. All caloric effects originate from the AFM/FM transition which encompasses changes in volume, magnetization, and entropy. The strong sensitivity of the transition temperatures to both hydrostatic pressure and magnetic field confers to this alloy outstanding values for the barocaloric and magnetocaloric strengths (|?S|/?p ~ 12 J kg-1K-1kbar-1 and |?S|/µ0?H~ 12 J kg-1K-1T-1). Both barocaloric and magnetocaloric effects have been found to be reproducible upon pressure and magnetic field cycling. Such a good reproducibility and the large caloric strengths make Fe-Rh alloys particularly appealing for solid-state cooling technologies at weak external stimuli.

Reversible adiabatic temperature changes at the magnetocaloric and barocaloric effects in Fe49Rh51

We report on the adiabatic temperature changes (ΔT) associated with the magnetocaloric and barocaloric effects in a Fe49Rh51 alloy. For the magnetocaloric effect, data derived from entropy curves are compared to direct thermometry measurements. The agreement between the two sets of data provides support to the estimation of ΔT for the barocaloric effect, which are indirectly determined from entropy curves. Large ΔT values are obtained at relatively low values of magnetic field (2 T) and hydrostatic pressure (2.5 kbar). It is also shown that both magnetocaloric and barocaloric effects exhibit good reproducibility upon magnetic field and hydrostatic pressure cycling, over a considerable temperature range.

Inverse barocaloric effects in ferroelectric BaTiO3 ceramics

We use calorimetry to identify pressure-driven isothermal entropy changes in ceramic samples of the prototypical ferroelectric BaTiO3. Near the structural phase transitions at ∼400 K (cubic-tetragonal) and ∼280 K (tetragonal-orthorhombic), the inverse barocaloric response differs in sign and magnitude from the corresponding conventional electrocaloric response. The differences in sign arise due to the decrease in unit-cell volume on heating through the transitions, whereas the differences in magnitude arise due to the large volumetric thermal expansion on either side of the transitions.

Ultrastable glasses portray similar behaviour to ordinary glasses at high pressure

Pressure experiments provide a unique opportunity to unravel new insights into glass-forming liquids by exploring its effect on the dynamics of viscous liquids and on the evolution of the glass transition temperature. Here we compare the pressure dependence of the onset of devitrification, Ton, between two molecular glasses prepared from the same material but with extremely different ambient-pressure kinetic and thermodynamic stabilities. Our data clearly reveal that, while both glasses exhibit different dTon/dP values at low pressures, they evolve towards closer calorimetric devitrification temperature and pressure dependence as pressure increases. We tentatively interpret these results from the different densities of the starting materials at room temperature and pressure. Our data shows that at the probed pressures, the relaxation time of the glass into the supercooled liquid is determined by temperature and pressure similarly to the behaviour of liquids, but using stability-dependent parameters.

Barocaloric and magnetocaloric effects in (MnNiSi)1−x(FeCoGe)x

(MnNiSi)1−x(FeCoGe)x undergoes a magnetostructural phase transition near room temperature that is acutely sensitive to applied hydrostatic pressure, which presents as a marked shift in the martensitic transition temperature (TM) by about –7.5 K/kbar. The magnetostructural transition can therefore be induced by applied hydrostatic pressure or by magnetic field. The barocaloric and magnetocaloric effects were measured across TM (for the sample with x = 0.38), and the corresponding entropy changes were +74 J/kg K (P = 2.7 kbar) and –58 J/kg K (μ0 H = 5 T), respectively. It was observed that the transition entropy change increases with pressure, which results in an enhancement of the barocaloric effect. Our measurements show that the transformed phase fraction associated with magnetostructural transition does not depend on pressure and, therefore, this enhancement cannot be attributed to a pressure-assisted completion of the phase transformation.

Modelling Shape-Memory Effects in Ferromagnetic Alloys

We develop a combined Ginzburg–Landau/micromagnetic model dealing with conventional and magnetic shape-memory properties in ferromagnetic shape-memory materials. The free energy of the system is written as the sum of structural, magnetic and magnetostructural contributions. We first analyse a mean field linearized version of the model that does not take into account long-range terms arising from elastic compatibility and demagnetization effects. This model can be solved analytically and in spite of its simplicity allows us to understand the role of the magnetostructural term in driving magnetic shape-memory effects. Numerical simulations of the full model have also been performed. They show that the model is able to reproduce magnetostructural microstructures reported in magnetic shape-memory materials such as Ni2MnGa as well as conventional and magnetic shape-memory behaviour.

Intermittent dynamics in externally driven ferroelastics and strain glasses

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Polymorphism of spironolactone: An unprecedented case of monotropy turning to enantiotropy with a huge difference in the melting temperatures

ABSTRACT Spironolactone form I melts at about 70 degrees lower than form II, which is very unusual for two co‐existing polymorphs. The phase relationships involving this unprecedented case of dimorphism have been investigated by constructing a topological pressure‐temperature phase diagram. The transition from polymorph I to polymorph II is unambiguously exothermic while it is accompanied with an increase in the specific volume. This indicates that the dP/dT slope of the I‐II equilibrium curve is negative. The convergence of the melting equilibrium lines at high pressure leads to a topological P‐T diagram in which polymorph I possesses a stable phase region at high pressure. Thus, forms I and II are monotropically related at ordinary pressure and turn to an enantiotropic relationship at high pressure. Given that polymorph I is the densest form, it negates the rule of thumb that the densest form is also the most stable form at room temperature, similar to the case of paracetamol.