Neutron spectroscopy measurements reveal short-range spin correlations near and above the ferromagnetic-paramagnetic phase transition in manganite materials of the form La$_{1-x}A_{x}$MnO$_{3}$, including samples with an insulating ground state as well as colossal magnetoresistive samples with a metallic ground state. Quasielastic magnetic scattering is revealed that forms clear ridges running along the [100]-type directions in momentum space. A simple model consisting of a conduction electron hopping between spin polarized Mn ions that becomes self-trapped after a few hops captures the essential physics of this magnetic component of the scattering. We associate this scattering component with the magnetic part of diffuse polarons, as we observe a temperature dependence similar to that of the diffuse structural scattering arising from individual polarons.
We report thermal-expansion, lattice-constant, and specific-heat data of the series La_1-xA_xCoO_3 for 0<= x <= 0.30 with A = Ca, Sr, and Ba. For the undoped compound LaCoO_3 the thermal-expansion coefficient alpha(T) exhibits a pronounced maximum around T=50K caused by a temperature-driven spin-state transition from a low-spin state of the Co^{3+$ ions at low towards a higher spin state at higher temperatures. The partial substitution of the La^{3+} ions by divalent Ca^{2+}, Sr^{2+}, or Ba^{2+} ions causes drastic changes in the macroscopic properties of LaCoO3. The large maximum in alpha(T) is suppressed and completely vanishes for x> 0.12. For A = Ca three different anomalies develop in alpha(T) with further increasing x, which are visible in specific-heat data as well. Together with temperature-dependent x-ray data we identify several phase transitions as a function of the doping concentration x and temperature. From these data we propose an extended phase diagram for La_1-xCa_xCoO_3.
We report on an a $mu$SR and $^{55}$Mn NMR investigation of the magnetic order parameter as a function of temperature in the optimally doped La$_{5/8}$(Ca$_y$Sr$_{1-y}$)$_{3/8}$MnO$_3$ and in the underdoped La$_{1-x}$Sr$_{x}$MnO$_3$ and La$_{1-x}$Ca$_{x}$MnO$_3$ metallic manganite families. The study is aimed at unraveling the effect of lattice distortions, implicitly controlled by the Ca-Sr isoelectronic substitution, from that of hole doping $x$ on the Curie temperature $T_c$ and the order of the magnetic transition. At optimal doping, the transitions are second order at all $y$ values, including the $y=1$ (La$_{5/8}$Ca$_{3/8}$MnO$_3$) end member. In contrast, they are first order in the underdoped samples, which show a finite (truncated) order parameter at the Curie point, including La$_{0.75}$Sr$_{0.25}$MnO$_3$ whose $T_c$ is much higher than that of La$_{5/8}$Ca$_{3/8}$MnO$_3$. The order parameter curves, on the other hand, exhibit a very minor dependence on $x$, if truncation is excepted. This suggests that the effective exchange interaction between Mn ions is essentially governed by local distortions, in agreement with the original double-exchange model, while truncation is primarily, if not entirely, an effect of under- or overdoping. A phase diagram, separating in the $x-y$ plane polaron-driven first order transitions from regular second order transitions governed by critical fluctuations, is proposed for the La$_{1-x}($Ca$_y$Sr$_{1-y}$)$_{x}$MnO$_3$ system.
We present a phenomenological theory for the ferromagnetic transition temperature, the magnetic susceptibility at high temperatures, and the structural distortion in the La$_{1-y}$(Ca$_{1-x}$Sr$_{x}$)$_{y}$MnO$_{3}$ system. We construct a Ginzburg-Landau free energy that describes the magnetic and the structural transitions, and a competition between them. The parameters of the magnetic part of the free energy are derived from a mean-field solution of the magnetic interaction for arbitrary angular momentum. The theory provides a qualitative description of the observed magnetic and structural phase transitions as functions of Sr-doping level ($x$) for $y=0.25$.
A laboratory hard X-ray photoelectron spectroscopy (HXPS) system equipped with a monochromatic Cr K$alpha$ ($h u = 5414.7$ eV) X-ray source was applied to an investigation of the core-level electronic structure of La$_{1-x}$Sr$_x$MnO$_3$. No appreciable high binding-energy shoulder in the O $1s$ HXPS spectra were observed while an enhanced low binding-energy shoulder structure in the Mn $2p_{3/2}$ HXPS spectra were observed, both of which are manifestation of high bulk sensitivity. Such high bulk sensitivity enabled us to track the Mn $2p_{3/2}$ shoulder structure in the full range of $x$, giving us a new insight into the binding-energy shift of the Mn $2p_{3/2}$ core level. Comparisons with the results using the conventional laboratory XPS ($h u = 1486.6$ eV) as well as those using a synchrotron radiation source ($h u = 7939.9$ eV) demonstrate that HXPS is a powerful and convenient tool to analyze the bulk electronic structure of a host of different compounds.
We report on Raman scattering measurements of single crystalline La$_{1-x}$Sr$_x$MnO$_3$ ($x$=0, 0.06, 0.09 and 0.125), focusing on the high frequency regime. We observe multi-phonon scattering processes up to fourth-order which show distinct features: (i) anomalies in peak energy and its relative intensity and (ii) a pronounced temperature-, polarization-, and doping-dependence. These features suggest a mixed orbiton-phonon nature of the observed multi-phonon Raman spectra.
Joel S. Helton
,Daniel M. Pajerowski
,Yiming Qiu
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(2014)
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"Polaron-mediated spin correlations in metallic and insulating La$_{1-x}A_{x}$MnO$_{3}$ ($A$=Ca, Sr, or Ba)"
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Joel Helton
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