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Register a new userStrain-mediated metal-insulator transition in epitaxial ultra-thin films of NdNiO3
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We have synthesized epitaxial NdNiO$_{3}$ ultra-thin films in a layer-by-layer growth mode under tensile and compressive strain on SrTiO$_{3}$ (001) and LaAlO$_3$ (001), respectively. A combination of X-ray diffraction, temperature dependent resistivity, and soft X-ray absorption spectroscopy has been applied to elucidate electronic and structural properties of the samples. In contrast to the bulk NdNiO$_{3}$, the metal-insulator transition under compressive strain is found to be completely quenched, while the transition remains under the tensile strain albeit modified from the bulk behavior.
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Ultrathin epitaxial films of EuNiO3 were grown on a series of substrates traversing highly compressive (- 2.4%) to highly tensile (2.5%) lattice mismatch. X-ray diffraction measurements showed the expected c-lattice parameter shift for compressive strain, but no detectable shift for tensilely strained substrates, while reciprocal space mapping confirmed the tensile strained film maintained epitaxial coherence. Transport measurements showed a successively (from tensile to compressive) lower resistance and a complete suppression of the metalinsulator transition at highly compressive lattice mismatch. Corroborating these findings, X-ray absorption spectroscopy measurements revealed a strong multiplet splitting in the tensile samples that progressively weakens with increasing compressive strain that, combined with cluster calculations, showed enhanced covalence between Ni-d and O-p orbitals leads to the metallic state.
Bulk NdNiO3 exhibits a metal-to-insulator transition (MIT) as the temperature is lowered that is also seen in tensile strained films. In contrast, films that are under a large compressive strain typically remain metallic at all temperatures. To clarify the microscopic origins of this behavior, we use position averaged convergent beam electron diffraction in scanning transmission electron microscopy to characterize strained NdNiO3 films both above and below the MIT temperature. We show that a symmetry lowering structural change takes place in case of the tensile strained film, which undergoes an MIT, but is absent in the compressively strained film. Using space group symmetry arguments, we show that these results support the bond length disproportionation model of the MIT in the rare-earth nickelates. Furthermore, the results provide insights into the non-Fermi liquid phase that is observed in films for which the MIT is absent.
Metal-insulator transition features as a transformation, from a highly charge conductive state to another state where charge conductivity is greatly suppressed when decreasing the temperature. Here we demonstrate two consecutive transitions in NdNiO3 films with CoFe2O4 capping, in which the metal-insulator transition occurs at 85 K, followed by an unprecedented insulator-metal transition below 40 K. The emerging insulator-metal transition associated with a weak antiferromagnetic behavior is observed in 20 unit cell-thick NdNiO3 with more than 5 unit cell CoFe2O4 capping. Differently, the NdNiO3 films with thinner CoFe2O4 capping only exhibit metal-insulator transition at 85 K, accompanied by a strong antiferromagnetic state below 40 K. Charge transfer from Co to Ni, instead of from Fe to Ni, formulates the ferromagnetic interaction between Ni-Ni and Ni-Co atoms, thus suppressing the antiferromagnetic feature and producing metallic conductive behavior. Furthermore, a phase diagram for the metal-insulator-metal transition in this system is drawn.
We have investigated the evolution of the electronic properties of La1-xSrxCrO3 (for the full range of x) epitaxial films deposited by molecular beam epitaxy (MBE) using x-ray diffraction, x-ray photoemission spectroscopy, Rutherford backscattering spectrometry, x-ray absorption spectroscopy, electrical transport, and ab initio modeling. LaCrO3 is an antiferromagnetic insulator whereas SrCrO3 is a metal. Substituting Sr2+ for La3+ in LaCrO3 effectively dopes holes into the top of valence band, leading to Cr4+ (3d2) local electron configurations. Core-level and valence-band features monotonically shift to lower binding energy with increasing x, indicating downward movement of the Fermi level toward the valence band maximum. The material becomes a p-type semiconductor at lower doping levels and an insulator-to-metal transition is observed at x greater than or equal to 0.65, but only when the films are deposited with in-plane compression via lattice-mismatched heteroepitaxy. Valence band x-ray photoemission spectroscopy reveals diminution of electronic state density at the Cr 3d t2g-derived top of the valence band while O K-edge x-ray absorption spectroscopy shows the development of a new unoccupied state above the Fermi level as holes are doped into LaCrO3. The evolution of these bands with Sr concentration is accurately captured using density functional theory with a Hubbard U correction of 3.0 eV (DFT + U). Resistivity data in the semiconducting regime (x less than or equal to 0.50) do not fit perfectly well to either a polaron hopping or band conduction model, but are best interpreted in terms of a hybrid model. The activation energies extracted from these fits are well reproduced by DFT + U.
In the perovskite oxide SrCrO$_{3}$ the interplay between crystal structure, strain and orbital ordering enables a transition from a metallic to an insulating electronic structure under certain conditions. We identified a narrow window of oxygen partial pressure in which highly strained SrCrO$_{3}$ thin films can be grown using radio-frequency (RF) off-axis magnetron sputtering on three different substrates, (LaAlO$_{3}$)$_{0.3}$-(Sr$_{2}$TaAlO$_{6}$)$_{0.7}$ (LSAT), SrTiO$_{3}$ (STO) and DyScO$_{3}$ (DSO). X-ray diffraction and atomic force microscopy confirmed the quality of the films and a metal-insulator transition driven by the substrate induced strain was demonstrated.
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