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Register a new userSuppression of spin-state transition in epitaxially strained LaCoO_{3}
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Epitaxial thin films of LaCoO_{3} (E-LCO) exhibit ferromagnetic order with a transition temperature T_c = 85 K, while polycrystalline thin LaCoO_{3} films (P-LCO) remain paramagnetic. The temperature-dependent spin-state structure for both E-LCO and P-LCO was studied by x-ray absorption spectroscopy at the Co L_{2,3} and O K edges. Considerable spectral redistributions over temperature are observed for P-LCO. The spectra for E-LCO, on the other hand, do not show any significant changes for temperatures between 30 K and 450 K at both edges, indicating that the spin state remains constant and that the epitaxial strain inhibits any population of the low-spin (S = 0) state with decreasing temperature. This observation identifies an important prerequisite for ferromagnetism in E-LCO thin films.
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Using soft x-ray absorption spectroscopy and magnetic circular dichroism at the Co-$L_{2,3}$ edge we reveal that the spin state transition in LaCoO$_{3}$ can be well described by a low-spin ground state and a triply-degenerate high-spin first excited state. From the temperature dependence of the spectral lineshapes we find that LaCoO$_{3}$ at finite temperatures is an inhomogeneous mixed-spin-state system. Crucial is that the magnetic circular dichroism signal in the paramagnetic state carries a large orbital momentum. This directly shows that the currently accepted low-/intermediate-spin picture is at variance. Parameters derived from these spectroscopies fully explain existing magnetic susceptibility, electron spin resonance and inelastic neutron data.
We report a magnetostriction study of a perovskite $rm{LaCoO}_{3}$ above 100 T using our state-of-the-art strain gauge to investigate an interplay between electron correlations and spin crossover. There has been a controversy regarding whether two novel phases in $rm{LaCoO}_{3}$ at high magnetic fields result from crystallizations or Bose-Einstein condensation during spin crossover as manifestations of localization and delocalization in spin states, respectively. We show that both phases are crystallizations rather than condensations, and the two crystallizations are different, based on the observations that the two phases exhibit as magnetostriction plateaux with distinct heights. The crystallizations of spin states have emerged manifesting the localizations and interactions in spin crossover with large and cooperative lattice changes.
A quantitative mathematical model for the critical thickness of strained epitaxial metal films is presented, at which the magnetic moment experiences a reorientation from in-plane to perpendicular magnetic anisotropy. The model is based on the minimum of the magnetic anisotropy energy with respect to the orientation of the magnetic moment of the film. Magnetic anisotropy energies are taken as the sum of shape anisotropy, magnetocrystalline anisotropy and magnetoelastic anisotropy, the two latter ones being present as constant surface and variable volume contributions. Other than anisotropy materials constants, readily available from literature, only information about the strain in the films for the determination of the magnetoelastic anisotropy energy is required. Application of the epitaxial Bain path allows to express the strain in the film in terms of substrate lattice constant and film lattice parameter, and thus to obtain an approximate closed expression for the reorientation thickness in terms of lattice mismatch. The model can predict the critical spin reorientation transition thickness with surprising accuracy.
The thermal expansion and heat capacity of FeSb2 at ambient pressure agrees with a picture of a temperature induced spin state transition within the Fe t_{2g} multiplet. However, high pressure powder diffraction data show no sign of a structural phase transition up to 7GPa. A bulk modulus B=84(3)GPa has been extracted and the temperature dependence of the Gruneisen parameter has been determined. We discuss here the relevance of a Kondo insulator description for this material.
Spin-state transition, also known as spin crossover, plays a key role in diverse systems, including minerals and biological materials. In theory, the boundary range between the low- and high-spin states is expected to enrich the transition and give rise to unusual physical states. However, no compound that realizes a nearly degenerate critical range as the ground state without requiring special external conditions has yet been experimentally identified. This study reports that, by comprehensive measurements of macroscopic physical properties, X-ray diffractometry, and neutron spectroscopy, the Sc substitution in LaCoO$_3$ destabilizes its nonmagnetic low-spin state and generates an anomalous paramagnetic state accompanied by the enhancement of transport gap and magneto-lattice-expansion as well as the contraction of Co--O distance with the increase of electron site-transfer. These phenomena are not well described by the mixture of conventional low- and high-spin states, but by their quantum superposition occurring on the verge of a spin-state transition. The present study enables us to significantly accelerate the design of new advanced materials without requiring special equipment based on the concept of quantum spin-state criticality.
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