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Register a new userMetal-insulator transition and electrically-driven memristive characteristics of SmNiO3 thin films
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The correlated oxide SmNiO3 (SNO) exhibits an insulator to metal transition (MIT) at 130 {deg}C in bulk form. We report on synthesis and electron transport in SNO films deposited on LaAlO3 (LAO) and Si single crystals. X-ray diffraction studies show that compressively strained single-phase SNO grows epitaxially on LAO while on Si, mixed oxide phases are observed. MIT is observed in resistance-temperature measurements in films grown on both substrates, with charge transport in-plane for LAO/SNO films and out-of-plane for Si/SNO films. Electrically-driven memristive behavior is realized in LAO/SNO films, suggesting that SNO may be relevant for neuromorphic devices.
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Heteroepitaxy offers a new type of control mechanism for the crystal structure, the electronic correlations, and thus the functional properties of transition-metal oxides. Here, we combine electrical transport measurements, high-resolution scanning transmission electron microscopy (STEM), and density functional theory (DFT) to investigate the evolution of the metal-to-insulator transition (MIT) in NdNiO$_3$ films as a function of film thickness and NdGaO$_3$ substrate crystallographic orientation. We find that for two different substrate facets, orthorhombic (101) and (011), modifications of the NiO$_6$ octahedral network are key for tuning the transition temperature $T_{text{MIT}}$ over a wide temperature range. A comparison of films of identical thickness reveals that growth on [101]-oriented substrates generally results in a higher $T_{text{MIT}}$, which can be attributed to an enhanced bond-disproportionation as revealed by the DFT+$U$ calculations, and a tendency of [011]-oriented films to formation of structural defects and stabilization of non-equilibrium phases. Our results provide insights into the structure-property relationship of a correlated electron system and its evolution at microscopic length scales and give new perspectives for the epitaxial control of macroscopic phases in metal-oxide heterostructures.
Cobaltates have rich spin-states and diverse properties. Using spin-state pictures and firstprinciples calculations, here we study the electronic structure and magnetism of the mixed-valent double perovskite YBaCo2O6. We find that YBaCo2O6 is in the formal intermediate-spin (IS) Co3+/low-spin (LS) Co4+ ground state. The hopping of eg electron from IS-Co3+ to LS-Co4+ via double exchange gives rise to a ferromagnetic half-metallicity, which well accounts for the recent experiments. The reduction of both magnetization and Curie temperature by oxygen vacancies is discussed, aided with Monte Carlo simulations. We also explore several other possible spin-states and their interesting electronic/magnetic properties. Moreover, we predict that a volume expansion more than 3% would tune YBaCo2O6 into the high-spin (HS) Co3+/LS Co4+ ferromagnetic state and simultaneously drive a metal-insulator transition. Therefore, spin-states are a useful parameter for tuning the material properties of cobaltates.
Magnetite (Fe$_{3}$O$_{4}$), an archetypal transition metal oxide, has been used for thousands of years, from lodestones in primitive compasses[1] to a candidate material for magnetoelectronic devices.[2] In 1939 Verwey[3] found that bulk magnetite undergoes a transition at T$_{V}$ $approx$ 120 K from a high temperature bad metal conducting phase to a low-temperature insulating phase. He suggested[4] that high temperature conduction is via the fluctuating and correlated valences of the octahedral iron atoms, and that the transition is the onset of charge ordering upon cooling. The Verwey transition mechanism and the question of charge ordering remain highly controversial.[5-11] Here we show that magnetite nanocrystals and single-crystal thin films exhibit an electrically driven phase transition below the Verwey temperature. The signature of this transition is the onset of sharp conductance switching in high electric fields, hysteretic in voltage. We demonstrate that this transition is not due to local heating, but instead is due to the breakdown of the correlated insulating state when driven out of equilibrium by electrical bias. We anticipate that further studies of this newly observed transition and its low-temperature conducting phase will shed light on how charge ordering and vibrational degrees of freedom determine the ground state of this important compound.
It was recently reported that a continuous electric current is a powerful control parameter to trigger changes in the electronic structure and metal-insulator transitions (MITs) in Ca2RuO4. However, the spatial evolution of the MIT and the implications of the unavoidable Joule heating have not been clarified yet, often hindered by the difficulty to asses the local sample temperature. In this work, we perform infrared thermal imaging on single-crystal Ca2RuO4 while controlling the MIT by electric current. The change in emissivity at the phase transition allows us to monitor the gradual formation and expansion of metallic phase upon increasing current. Our local temperature measurements indicate that, within our experimental resolution, the MIT always occurs at the same local transition temperatures, irrespectively if driven by temperature or by current. Our results highlight the importance of local heating, phase coexistence, and microscale inhomogeneity when studying strongly correlated materials under the flow of electric current.
Impedance spectroscopy measurements were performed in high quality Vanadium dioxide (VO2) thin films. This technique allows us investigate the resistive and capacitive contribution to the dielectric response near the metal-insulator transition (MIT). A non ideal RC behavior was found in our films from room temperature up to 334 K. A decrease of the total capacitance was found in this region, possibly due to interface effects. Above the MIT, the system behaves like a metal as expected, and a modified equivalent circuit is necessary to describe the impedance data adequately. Around the MIT, an increase of the total capacitance is observed.
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