We have investigated the change in entropy with direct measurements of heat flow as a function of magnetic field at fixed temperatures across the entire phase diagram of the phase-separated (PS) compound La$_{0.25}$Pr$_{0.375}$Ca$_{0.375}$MnO$_3$ (LPCMO). At this composition, the compound shows competing charge-ordered/antiferromagnetic (CO/AF) ground states. At a fixed temperature, we observe an increase in hysteresis in the entropy as a function of the applied field. The heat flux shows progressively irreversible hysteresis, which characterizes the energy barriers between the two competing ground states, as the temperature is lowered. The increase in the heat loss correlates with the increase in magnetic viscosity in the phase-separated state. Keywords: manganites, avalanche effect, phase transition, heat flow, DSC, entropy. Corresponding author: [email protected] . On 10 April 2020, this JAC-Elsevier article was accepted. Yet, its online publication shows numerous errors: Cut-off text, missing Figure Captions, incomplete Table ... None of which is our fault! This makes our paper hard to read, study and/or understand. This reproduction is our final (error-free!) revision. When citing our refereed paper, please also refer to this arXiv print. Thank you for understanding
We have studied the irreversibility of the magnetization induced by thermal cycles in La0.5Ca0.5MnO3 manganites, which present a low temperature state characterized by the coexistence of phases. The effect is evidenced by a decrease of the magnetization after cycling the sample between 300 and 50 K. We developed a phenomenological model that allows us to correlate the value of the magnetization with the number of cycles performed. The experimental results show excellent agreement with our model, suggesting that this material could be used for the development of a device to monitor thermal changes. The effect of thermal cycling is towards an increase of the amount of the non ferromagnetic phase in the compounds and it might be directly related with the strain at the contact surface among the coexisting phases.
We have studied magnetic and transport properties on different manganese oxide based compounds exhibiting phase separation: polycrystalline La5/8-yPryCa3/8MnO3 (y=0.3) and La1/2Ca1/2Mn1-zFezO3 (z = 0.05), and single crystals of La5/8-yPryCa3/8MnO3 (y=0.35). Time dependent effects indicate that the fractions of the coexisting phases are dynamically changing in a definite temperature range. We found that in this range the ferromagnetic fraction f can be easily tuned by application of low magnetic fields (< 1 T). The effect is persistent after the field is turned off, thus the field remains imprinted in the actual value of f and can be recovered through transport measurements. This effect is due both to the existence of a true phase separated equilibrium state with definite equilibrium fraction f0, and to the slow growth dynamics. The fact that the same global features were found on different compounds and in polycrystalline and single crystalline samples, suggests that the effect is a general feature of some phase separated media.
Substitutions in the Mn-sublattice of antiferromagnetic, charge and orbitally ordered manganites was recently found to produce intriguing metamagnetic transitions, consisting of a succession of sharp magnetization steps separated by plateaus. The compounds exhibiting such features can be divided in two categories, depending on whether they are sensitive to thermal cycling effects or not. One compound of each category has been considered in the present study. The paper reports on the influence of two treatments: high-temperature annealing and grinding. It is shown that both of these treatments can drastically affect the phenomenon of magnetization steps. These results provide us with new information about the origin of these jumps in magnetization.
We have studied the effect of irreversibility induced by repeated thermal cycles on the electric transport and magnetization of polycrystalline samples of La0.5Ca0.5MnO3 and La0.325Pr0.3Ca0.375MnO3. An increase of the resistivity and a decrease of the magnetization at different temperature ranges after cycling is obtained in the temperature range between 300 K and 30 K. Both compounds are known to exhibit intrinsic submicrometric coexistence of phases and undergo a sequence of phase transitions related to structural changes. Changes induced by thermal cycling can be partially inhibited by applying magnetic field and hydrostatic pressure. Our results suggest that the growth and coexistence of phases with different structures gives rise to microstructural tracks and strain accommodation, producing the observed irreversibility. Irrespective of the actual ground state of each compound, the effect of thermal cycling is towards an increase of the amount of the insulating phase in both compounds.
We present a phenomenological model based on the thermodynamics of the phase separated state of manganites, accounting for its static and dynamic properties. Through calorimetric measurements on La$_{0.225}$Pr$_{0.40}$Ca$ _{0.375}$MnO$_{3}$ the low temperature free energies of the coexisting ferromagnetic and charge ordered phases are evaluated. The phase separated state is modeled by free energy densities uniformly spread over the sample volume. The calculations contemplate the out of equilibrium features of the coexisting phase regime, to allow a comparison between magnetic measurements and the predictions of the model. A phase diagram including the static and dynamic properties of the system is constructed, showing the existence of blocked and unblocked regimes which are characteristics of the phase separated state in manganites.
A.L. Lima-Sharma Sandian National Laboratories
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(2020)
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"Irreversible Heat Flow Across Phase Boundaries in Phase-Separated Manganites"
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Carolus Boekema
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