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Register a new userMechanism and Control Parameters of the Coupled Structural and Metal-Insulator Transition in Nickelates
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Rare-earth nickelates exhibit a remarkable metal-insulator transition accompanied by a structural transition associated with a lattice `breathing mode. Using model considerations and first-principles calculations, we present a theory of this phase transition, which reveals the key role of the coupling between the electronic and lattice instabilities. We show that the transition is driven by the proximity to an electronic disproportionation instability which couples to the breathing mode, thus cooperatively driving the system into the insulating state. This allows us to identify two key control parameters of the transition: the susceptibility to electronic disproportionation and the stiffness of the lattice mode. We show that our findings can be rationalized in terms of a Landau theory involving two coupled order parameters, with general implications for transition-metal oxides.
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For most metals, increasing temperature (T) or disorder will quicken electron scattering. This hypothesis informs the Drude model of electronic conductivity. However, for so-called bad metals this predicts scattering times so short as to conflict with Heisenbergs uncertainty principle. Here we introduce the rare-earth nickelates (RNiO_3, R = rare earth) as a class of bad metals. We study SmNiO_3 thin films using infrared spectroscopy while varying T and disorder. We show that the interaction between lattice distortions and Ni-O bond covalence explains both the bad metal conduction and the insulator-metal transition in the nickelates by shifting spectral weight over the large energy scale established by the Ni-O orbital interaction, thus enabling very low sigma while preserving the Drude model and without violating the uncertainty principle.
Rare-earth nickelates exhibit a metal-insulator transition accompanied by a structural distortion that breaks the symmetry between formerly equivalent Ni sites. The quantitative theoretical description of this coupled electronic-structural instability is extremely challenging. Here, we address this issue by simultaneously taking into account both structural and electronic degrees of freedom using a charge self-consistent combination of density functional theory and dynamical mean-field theory, together with screened interaction parameters obtained from the constrained random phase approximation. Our total energy calculations show that the coupling to an electronic instability towards a charge disproportionated insulating state is crucial to stabilize the structural distortion, leading to a clear first order character of the coupled transition. The decreasing octahedral rotations across the series suppress this electronic instability and simultaneously increase the screening of the effective Coulomb interaction, thus weakening the correlation effects responsible for the metal-insulator transition. Our approach allows to obtain accurate values for the structural distortion and thus facilitates a comprehensive understanding, both qualitatively and quantitatively, of the complex interplay between structural properties and electronic correlation effects across the nickelate series.
The metal-insulator transition (MIT) of VO2 is discussed with particular emphasis on the structural instability of the rutile compounds toward dimerization. Ti substitution experiments reveal that the MIT is robust up to 20% Ti substitutions and occurs even in extremely thin V-rich lamellas in spinodally decomposed TiO2-VO2 composites, indicating that the MIT is insensitive to hole doping and essentially takes on a local character. These observations suggest that either electron correlation in the Mott-Hubbard sense or Peierls (Fermi-surface) instability plays a minor role on the MIT. Through a broad perspective of crystal chemistry on the rutile-related compounds, it is noted that VO2 and another MIT compound NbO2 in the family eventually lie just near the borderline between the two structural groups with the regular rutile structure and the distorted structures characterized by the formation of dimers with direct metal-metal bonding. The MITs of VO2 and NbO2 are natural consequences of structural transitions between the two groups, as all the d electrons are trapped in the bonding molecular orbitals of dimers at low temperatures. Such dimer crystals are ubiquitously found in early transition metal compounds having chain-like structures, such as MoBr3, NbCl4, Ti4O7, and V4O7, the latter two of which also exhibit MITs probably of the same origin. In a broader sense, the dimer crystal is a kind of molecular orbital crystals in which virtual molecules made of transition metal atoms with partially-filled t2g shells, such as dimers, trimers or larger ones, are generated by metal-metal bonding and are embedded into edge- or face-sharing octahedron networks of various kinds. The molecular orbital crystallization opens a natural route to stabilization of unpaired t2g electrons in crystals.
Nucleation processes of mixed-phase states are an intrinsic characteristic of first-order phase transitions, typically related to local symmetry breaking. Direct observation of emerging mixed-phase regions in materials showing a first-order metal-insulator transition (MIT) offers unique opportunities to uncover their driving mechanism. Using photoemission electron microscopy, we image the nanoscale formation and growth of insulating domains across the temperature-driven MIT in NdNiO3 epitaxial thin films. Heteroepitaxy is found to strongly determine the nanoscale nature of the phase transition, inducing preferential formation of striped domains along the terraces of atomically flat stepped surfaces. We show that the distribution of transition temperatures is an intrinsic local property, set by surface morphology and stable across multiple temperature cycles. Our data provides new insights into the MIT of heteroepitaxial nickelates and points to a rich, nanoscale phenomenology in this strongly correlated material.
We show that synthesis-induced Metal -Insulator transition (MIT) for electronic transport along the orthorombic c axis of FeSb$_{2}$ single crystals has greatly enhanced electrical conductivity while keeping the thermopower at a relatively high level. By this means, the thermoelectric power factor is enhanced to a new record high S$^{2}$$sigma$ $sim$ 8000 $mu$WK$^{-2}$cm$^{-1}$ at 28 K. We find that the large thermopower in FeSb$_{2}$ can be rationalized within the correlated electron model with two bands having large quasiparaticle disparity, whereas MIT is induced by subtle structural differences. The results in this work testify that correlated electrons can produce extreme power factor values.
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