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Register a new userGeometric influence on the net magnetic moment in LaCoO$_3$ thin films
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The different magnetic behaviors of LaCoO$_3$ films grown on LaAlO$_3$ and SrTiO$_3$ are related to the Co-O-Co bond angles and the constraints imposed on the Co-O bond lengths by the substrate geometries. Long-range magnetic order occurs below T ~ 90 K when the Co-O-Co bond angle is greater than 163 degrees, consistent with the behavior of bulk and nanoparticles forms of LaCoO$_3$. A LaAlO$_3$ substrate prevents magnetic long-range order at low temperatures near the film-substrate interface and collinear antiferromagnetic sublattices away from the interface. At low temperatures, the antiferromagnetically ordered sublattices are non-collinear in films grown on SrTiO$_3$ substrates, leading to a significant net moment.
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The spin states of Co$^{3+}$ ions in perovskite-type LaCoO$_3$, governed by complex interplay between the electron-lattice interactions and the strong electron correlations, still remain controversial due to the lack of experimental techniques which can detect directly. In this letter, we revealed the tensile-strain dependence of spin states, $i. e.$ the ratio of the high- and low-spin states, in epitaxial thin films and a bulk crystal of LaCoO$_3$ via resonant inelastic soft x-ray scattering. The tensile-strain as small as 1.0% was found to realize different spin states from that in the bulk.
We study ferromagnetic ordering and microscopic inhomogeneity in tensile strained LaCoO$_3$ using numerical simulations. We argue that both phenomena originate from effective superexchange interactions between atoms in the high-spin (HS) state mediated by the intermediate-spin excitations. We derive a model of the HS excitation as a bare atomic state dressed by electron and electron-hole fluctuations on the neighbor atoms. We construct a series of approximations to account for electron correlation effects responsible for HS fluctuations and magnetic exchange. The obtained amplitudes and directional dependence of magnetic couplings between the dressed HS states show a qualitative agreement with experimental observations and provide a new physical picture of LaCoO$_3$ films.
The effect of high tensile strain and low dimensionality on the magnetic and electronic properties of CaMnO$_3$ ultrathin films, epitaxially grown on SrTiO$_3$ substrates, are experimentally studied and theoretically analyzed. By means of ab initio calculations, we find that, both, the high strain produced by the substrate and the presence of the free surface contribute to the stabilization of an in-plane ferromagnetic coupling, giving rise to a non-zero net magnetic moment in the ultrathin films. Coupled with this change in the magnetic order we find an insulator-metal transition triggered by the quantum confinement and the tensile epitaxial strain. Accordingly, our magnetic measurements in 3nm ultrathin films show a ferromagnetic hysteresis loop, absent in the bulk compound due to its G-type antiferromagnetic structure.
Atomistic defect engineering through the pulsed laser epitaxy of perovskite transition metal oxides offers facile control of their emergent opto-electromagnetic and energy properties. Among the various perovskite oxides, EuTiO3 exhibits a strong coupling between the lattice, electronic, and magnetic degrees of freedom. This coupling is highly susceptible to atomistic defects. In this study, we investigated the magnetic phase of EuTiO$_3$ epitaxial thin films via systematic defect engineering. A magnetic phase transition from an antiferromagnet to a ferromagnet was observed when the unit cell volume of EuTiO3 expanded due to the introduction of Eu-O vacancies. Optical spectroscopy and density functional theory calculations show that the change in the electronic structure as the ferromagnetic phase emerges can be attributed to the weakened Eu-Ti-Eu super-exchange interaction and the developed ferromagnetic Eu-O-Eu interaction. Facile defect engineering in EuTiO$_3$ thin films facilitates understanding and tailoring of their magnetic ground state.
Cobalt nitride (Co-N) thin films prepared using a reactive magnetron sputtering process by varying the relative nitrogen gas flow (pn) are studied in this work. As pn~increases, Co(N), tcn, Co$_3$N and CoN phases are formed. An incremental increase in pn, after emergence of tcn~phase at pn=10p, results in a continuous expansion in the lattice constant ($a$) of tcn. For pn=30p, $a$ maximizes and becomes comparable to its theoretical value. An expansion in $a$ of tcn, results in an enhancement of magnetic moment, to the extent that it becomes even larger than pure Co. Though such higher (than pure metal) magnetic moment for Fe$_4$N thin films have been theoretically predicted and evidenced experimentally, higher (than pure Co) magnetic moment are evidenced in this work and explained in terms of large-volume high-moment model for tetra metal nitrides.
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