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Register a new userLow Temperature Magnetothermodynamics of Pr{0.7}Ca{0.3}MnO{3}
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Manojeet Bhattacharya
Publication date
2001
fields
Physics
and research's language is
English
Authors
M. Roy
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We present a detailed magnetothermal study of Pr$_{0.7}$Ca$_{0.3}$MnO$_{3}$, a perovskite manganite in which an insulator-metal transition can be driven by magnetic field, but also by pressure, visible light, x-rays, or high currents. We find that the field-induced transition is associated with a large release of energy which accounts for its strong irreversibility. In the ferromagnetic metallic state, specific heat and magnetization measurements indicate a much smaller spin wave stiffness than that seen in any other ferromagnetic manganite, which we explain in terms of ferromagnetism among the Pr moments. The Pr ferromagnetism also appears to influence the low temperature thermodynamic phase diagram of this material and the uniquely sensitive metastability of the insulating state.
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The family of hole-doped Pr-based perovskite cobaltites, Pr$_{0.5}$Ca$_{0.5}$CoO$_{3}$ and (Pr$_{1-y}$RE$_{y}$)$_{0.3}$Ca$_{0.7}$CoO$_{3}$ (where RE is rare earth) has recently been found to exhibit simultaneous metal-insulator, spin-state, and valence transitions. We have investigated magnetic-field-induced phase transitions of (Pr$_{1-y}$Y$_{y}$)$_{0.7}$Ca$_{0.3}$CoO$_{3}$ by means of magnetization measurements at 4.2$-$100 K up to an ultrahigh magnetic field of 140 T with the chemical pressure varied by $y$ = 0.0625, 0.075, 0.1. The observed magnetic-field-induced transitions were found to occur simultaneously with the metal-insulator transitions up to 100 T. The obtained magnetic field-temperature ($B$-$T$) phase diagram and magnetization curves are well analyzed by a spin-crossover model of a single ion with interion interactions. On the other hand, the chemical pressure dependence of the experimentally obtained magnetization change during the phase transition disagrees with the single ion model when approaching low temperatures. The significant $y$ dependence of the magnetization change at low temperatures may arise from the itinerant magnetism of Co$^{3+}$ in the paramagnetic metallic phase, where the chemical pressure enhances the exchange splitting by promoting the double-exchange interaction. The observed $B$-$T$ phase diagrams of (Pr$_{1-y}$Y$_{y}$)$_{0.7}$Ca$_{0.3}$CoO$_{3}$ are quite contrary to that of LaCoO$_{3}$, indicating that in (Pr$_{1-y}$Y$_{y}$)$_{0.7}$Ca$_{0.3}$CoO$_{3}$ the high-field phase possesses higher entropy than the low-field phase, whereas it is the other way around in LaCoO$_{3}$.
The structural and magnetic properties of two mixed-valence cobaltites with formal population of 0.30 Co$^{4+}$ ions per f.u., (Pr$_{1-y}$Y$_{y}$)$_{0.7}$Ca$_{0.3}$CoO$_3$ ($y=0$ and 0.15), have been studied down to very low temperatures by means of the high-resolution neutron diffraction, SQUID magnetometry and heat capacity measurements. The results are interpreted within the scenario of the spin-state crossover from a room-temperature mixture of the intermediate spin Co$^{3+}$ and low spin Co$^{4+}$ (IS/LS) at the to the LS/LS mixture in the sample ground states. In contrast to the yttrium free $y=0$ that retains the metallic-like character and exhibits ferromagnetic ordering below 55 K, the doped system $y=0.15$ undergoes a first-order metal-insulator transition at 132 K, during which not only the crossover to low spin states but also a partial electron transfer from Pr$^{3+}$ 4f to cobalt 3d states take place simultaneously. Taking into account the non-magnetic character of LS Co$^{3+}$, such valence shift electronic transition causes a magnetic dilution, formally to 0.12 LS Co$^{4+}$ or 0.12 $t_{2g}$ hole spins per f.u., which is the reason for an insulating, highly non-uniform magnetic ground state without long-range order. Nevertheless, even in that case there exists a relatively strong molecular field distributed over all the crystal lattice. It is argued that the spontaneous FM order in $y=0$ and the existence of strong FM correlations in $y=0.15$ apparently contradict the single $t_{2g}$ band character of LS/LS phase. The explanation we suggest relies on a model of the defect induced, itinerant hole mediated magnetism, where the defects are identified with the magnetic high-spin Co$^{3+}$ species stabilized near oxygen vacancies.
The electric, magnetic, and thermal properties of three perovskite cobaltites with the same 30% hole doping and ferromagnetic ground state were investigated down to very low temperatures. With decreasing size of large cations, the ferromagnetic Curie temperature and spontaneous moments of cobalt are gradually suppressed - $T_C=130$ K, 55 K and 25 K and $m = 0.68 mu_B$, 0.34 $mu_B$ and 0.23 $mu_B$ for Nd$_{0.7}$Sr$_{0.3}$CoO$_3$, Pr$_{0.7}$Ca$_{0.3}$CoO$_3$ and Nd$_{0.7}$Ca$_{0.3}$CoO$_3$, respectively. The moment reduction with respect to moment of the conventional ferromagnet La$_{0.7}$Sr$_{0.3}$CoO$_3$ ($T_C=230$ K, $m = 1.71 mu_B$) in so-called IS/LS state for Co$^{3+}$/Co$^{4+}$, was originally interpreted using phase-separation scenario. Based on the present results, mainly the analysis of Schottky peak originating in Zeeman splitting of the ground state Kramers doublet of Nd$^{3+}$, we find, however, that ferromagnetic phase in Nd$_{0.7}$Ca$_{0.3}$CoO$_3$ and likely also Pr$_{0.7}$Ca$_{0.3}$CoO$_3$ is uniformly distributed over all sample volume, despite the severe drop of moments. The ground state of these compounds is identified with the LS/LS-related phase derived theoretically by Sboychakov textit{et al.} [Phys. Rev. B textbf{80}, 024423 (2009)]. The ground state of Nd$_{0.7}$Sr$_{0.3}$CoO$_3$ with an intermediate cobalt moment is inhomogeneous due to competing of LS/LS and IS/LS phases. In the theoretical part of the study, the crystal field split levels for $4f^3$ (Nd$^{3+}$), $4f^2$ (Pr$^{3+}$) and $4f^1$ (Ce$^{3+}$ or Pr$^{4+}$) are calculated and their magnetic characteristics are presented.
The magnetic, electric and thermal properties of the ($Ln_{1-y}$Y$_{y}$)$_{0.7}$Ca$_{0.3}$CoO$_3$ perovskites ($Ln$~=~Pr, Nd) were investigated down to very low temperatures. The main attention was given to a peculiar metal-insulator transition, which is observed in the praseodymium based samples with $y=0.075$ and 0.15 at $T_{M-I}=64$ and 132~K, respectively. The study suggests that the transition, reported originally in Pr$_{0.5}$Ca$_{0.5}$CoO$_3$, is not due to a mere change of cobalt ions from the intermediate- to the low-spin states, but is associated also with a significant electron transfer between Pr$^{3+}$ and Co$^{3+}$/Co$^{4+}$ sites, so that the praseodymium ions occur below $T_{M-I}$ in a mixed Pr$^{3+}$/Pr$^{4+}$ valence. The presence of Pr$^{4+}$ ions in the insulating phase of the yttrium doped samples (Pr$_{1-y}$Y$_{y}$)$_{0.7}$Ca$_{0.3}$CoO$_3$ is evidenced by Schottky peak originating in Zeeman splitting of the ground state Kramers doublet. The peak is absent in pure Pr$_{0.7}$Ca$_{0.3}$CoO$_3$ in which metallic phase, based solely on non-Kramers Pr$^{3+}$ ions, is retained down to the lowest temperature.
Using ultrafast optical spectroscopy, we show that polaronic behavior associated with interfacial antiferromagnetic order is likely the origin of tunable magnetotransport upon switching the ferroelectric polarity in a La$_{0.7}$Ca$_{0.3}$MnO$_{3}$/BiFeO$_{3}$ (LCMO/BFO) heterostructure. This is revealed through the difference in dynamic spectral weight transfer between LCMO and LCMO/BFO at low temperatures, which indicates that transport in LCMO/BFO is polaronic in nature. This polaronic feature in LCMO/BFO decreases in relatively high magnetic fields due to the increased spin alignment, while no discernible change is found in the LCMO film at low temperatures. These results thus shed new light on the intrinsic mechanisms governing magnetoelectric coupling in this heterostructure, potentially offering a new route to enhancing multiferroic functionality.
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