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Register a new userThe metal-insulator transition and its relation to magnetic structure in (LaMnO3)2n/(SrMnO3)n superlattices
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Superlattices of (LaMnO3)2n/(SrMnO3)n (n=1 to 5), composed of the insulators LaMnO3 and SrMnO3, undergo a metal-insulator transition as a function of n, being metallic for n<=2 and insulating for n>=3. Measurements of transport, magnetization and polarized neutron reflectivity reveal that the ferromagnetism is relatively uniform in the metallic state, and is strongly modulated in the insulating state, being high in LaMnO3 and suppressed in SrMnO3. The modulation is consistent with a Mott transition driven by the proximity between the (LaMnO3)/(SrMnO3) interfaces. Disorder localizes states at the Fermi level at the interfaces for n>=3. We suggest that this disorder is due to magnetic frustration at the interfaces.
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The magnetic and electronic modifications induced at the interfaces in (SrMnO$_{3}$)$_{n}$/(LaMnO$_{3}$)$_{2n}$ superlattices have been investigated by linear and circular magnetic dichroism in the Mn L$_{2,3}$ x-ray absorption spectra. Together with theoretical calculations, our data demonstrate that the charge redistribution across interfaces favors in-plane ferromagnetic (FM) order and $e_{g}(x^{2}-y^{2})$ orbital occupation, in agreement with the average strain. Far from interfaces, inside LaMnO$_3$, electron localization and local strain favor antiferromagnetism (AFM) and $e_{g}(3z^{2}-r^{2})$ orbital occupation. For $n=1$ the high density of interfacial planes ultimately leads to dominant FM order forcing the residual AFM phase to be in-plane too, while for $n geq 5$ the FM layers are separated by AFM regions having out-of-plane spin orientation.
We measure the optical conductivity of (SrMnO3)n/(LaMnO3)2n superlattices (SL) for n=1,3,5, and 8 and 10 < T < 400 K. Data show a T-dependent insulator to metal transition (IMT) for n leq 3, driven by the softening of a polaronic mid-infrared band. At n = 5 that softening is incomplete, while at the largest-period n=8 compound the MIR band is independent of T and the SL remains insulating. One can thus first observe the IMT in a manganite system in the absence of the disorder due to chemical doping. Unsuccessful reconstruction of the SL optical properties from those of the original bulk materials suggests that (SrMnO3)n/(LaMnO3)2n heterostructures give rise to a novel electronic state.
The modulation of charge density and spin order in (LaMnO$_3$)$_{2n}$/(SrMnO$_3$)$_n$ ($n$=1-4) superlattices is studied via Monte Carlo simulations of the double-exchange model. G-type antiferromagnetic barriers in the SrMnO$_{3}$ regions with low charge density are found to separate ferromagnetic LaMnO$_{3}$ layers with high charge density. The recently experimentally observed metal-insulator transition with increasing $n$ is reproduced in our studies, and $n=3$ is found to be the critical value.
Calculations employing the local density approximation combined with static and dynamical mean-field theories (LDA+U and LDA+DMFT) indicate that the metal-insulator transition observed at 32 GPa in paramagnetic LaMnO3 at room temperature is not a Mott-Hubbard transition, but is caused by orbital splitting of the majority-spin eg bands. For LaMnO3 to be insulating at pressures below 32 GPa, both on-site Coulomb repulsion and Jahn-Teller distortion are needed.
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.
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