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We report on calorimetry under applied hydrostatic pressure and magnetic field at the antiferromagnetic (AFM)-ferromagnetic (FM) transition of Fe$_{49}$Rh$_{51}$. Results demonstrate the existence of a giant barocaloric effect in this alloy, a new 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 ($|Delta S|$/$Delta p$ $sim$ 12 J kg$^{-1}$ K $^{-1}$ kbar$^{-1}$ and $|Delta S|$/$mu_0Delta H$ $sim$ 12 J kg$^{-1}$ K$^{-1}$ T$^{-1}$). 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.
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There is currently great interest in replacing the harmful volatile hydrofluorocarbon fluids used in refrigeration and air-conditioning with solid materials that display magnetocaloric, electrocaloric or mechanocaloric effects. However, the field-driven thermal changes in all of these caloric materials fall short with respect to their fluid counterparts. Here we show that plastic crystals of neopentylglycol (CH3)2C(CH2OH)2 display unprecedentedly large pressure-driven thermal changes near room temperature due to molecular reconfiguration, and that these changes are comparable with those exploited commercially in hydrofluorocarbons. Our discovery of colossal barocaloric effects in a plastic crystal should bring barocaloric materials to the forefront of research and development in order to achieve safe environmentally friendly cooling without compromising performance.
Nowadays the world is facing a prominent paradox regarding thermal energy. The production of heat accounts for more than 50% of global final energy consumption while the waste heat potential analysis reveals that 72% of the global primary energy consumption is lost after conversion mainly in the form of heat. Towards global decarbonization, it is of vital importance to establish a solution to thermal energy utilization under full control. Here, we propose and realize an unprecedented concept -- barocaloric thermal batteries based on the inverse colossal barocaloric effect of NH4SCN. Thermal charging is initialized upon pressurization through an order-to-disorder phase transition below 364 K and in turn the discharging of 43 J g-1, which are eleven times more than the input mechanical energy, occurs on demand at depressurization at lower temperatures. The discharging is also manifested as a directly measured temperature rise of 12 K. The thermodynamic equilibrium nature of the pressure-restrained heat-carrying phase guarantees stable storage and/or transport over a variety of temporal and/or spatial scales. The barocaloric thermal batteries reinforced by their solid microscopic mechanism are expected to significantly advance the ability to take advantage of waste heat.
Physical nature of giant magnetocaloric and electrocaloric effects, MCE and ECE, is explained in terms of the new fundamentals of phase transitions, ferromagnetism and ferroelectricity. It is the latent heat of structural (nucleation-and-growth) phase transitions from a normal crystal state to the orientation-disordered crystal (ODC) state where the constituent particles are engaged in thermal rotation. The ferromagnetism or ferroelectricity of the material provides the capability to trigger the structural phase transition by application, accordingly, of magnetic or electric field.
The structural phase transitions of MF$_3$ (M=Al, Cr, V, Fe, Ti, Sc) metal trifluorides are studied within a simple Landau theory consisting of tilts of rigid MF$_6$ octahedra associated with soft antiferrodistoritive optic modes that are coupled to long-wavelength strain generating acoustic phonons. We calculate the temperature and pressure dependence of several quantities such as the spontaneous distortions, volume expansion and shear strains as well as $T-P$ phase diagrams. By contrasting our model to experiments we quantify the deviations from mean-field behavior and found that the tilt fluctuations of the MF$_6$ octahedra increase with metal cation size. We apply our model to predict giant barocaloric effects in Sc substituted TiF$_3$ of up to about $15,$JK$^{-1}$kg$^{-1}$ for modest hydrostatic compressions of $0.2,$GPa. The effect extends over a wide temperature range of over $140,$K (including room temperature) due to a large predicted rate $dT_c/dP = 723,$K GPa$^{-1}$, which exceeds those of typical barocaloric materials. Our results suggest that open lattice frameworks such as the trifluorides are an attractive platform to search for giant barocaloric effects.
Combining multiple degrees of freedom in strongly-correlated materials such as transition-metal oxides would lead to fascinating magnetic and magnetocaloric features. Herein, the strain effects are used to markedly tailor the magnetic and magnetocaloric properties of PrVO3 thin films. The selection of appropriate thickness and substrate enables us to dramatically decrease the coercive magnetic field from 2.4 T previously observed in sintered PVO3 bulk to 0.05 T for compressive thin films making from the PrVO3 compound a nearly soft magnet. This is associated with a marked enhancement of the magnetic moment and the magnetocaloric effect that reach unusual maximum values of roughly 4.86 uB and 56.8 J/kg K in the magnetic field change of 6 T applied in the sample plane at the cryogenic temperature range (3 K), respectively. This work strongly suggests that taking advantage of different degrees of freedom and the exploitation of multiple instabilities in a nanoscale regime is a promising strategy for unveiling unexpected phases accompanied by a large magnetocaloric effect in oxides.
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