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Particle-hole asymmetric lifetimes promoted by spin and orbital fluctuations in ultrahin SrVO$_3$ films

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 Added by Matthias Pickem
 Publication date 2020
  fields Physics
and research's language is English




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The multi-orbital Hubbard model is known to host various ordered states such as antiferromagnetism, ferromagnetism and orbital-order. Here we propose an engineered system - an ultrathin SrVO$_3$ film - to realize all said orders upon carrier doping, achievable with realistic gate-voltages. As a central observation we find that throughout the phase diagram, dominant non-local fluctuations lead to a momentum differentiation of the self-energy, particularly the scattering rate. In contrast to the pseudogap behavior in the one-band Hubbard model, here in the multi-band case the differentiation is between momenta on the occupied and unoccupied side of the Fermi surface. Our work, based on the dynamical vertex approximation, hence complements the understanding of spectral signatures of nearby second order phase transitions and calls to reexamine the momentum differentiation in other systems using methods beyond dynamical mean-field theory.



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Oxygen packaging in transition metal oxides determines the metal-oxygen hybridization and electronic occupation at metal orbitals. Strontium vanadate (SrVO$_3$), having a single electron in a $3d$ orbital, is thought to be the simplest example of strongly correlated metallic oxides. Here, we determine the effects of epitaxial strain on the electronic properties of SrVO$_3$ thin films, where the metal-oxide sublattice is corner-connected. Using x-ray absorption and x-ray linear dichroism at the V $L_{2,3}$ and O $K$-edges, it is observed that tensile or compressive epitaxial strain change the hierarchy of orbitals within the $t_{2g}$ and $e_g$ manifolds. Data show a remarkable $2p-3d$ hybridization, as well as a strain-induced reordering of the V $3d$($t_{2g}$, $e_g$) orbitals. The latter is itself accompanied by a consequent change of hybridization that modulates the hybrid $pi^*$ and $sigma^*$ orbitals and the carrier population at the metal ions, challenging a rigid band picture.
In systems where electrons form both dispersive bands and small local spins, we show that changes of the spin configuration can tune the bands through a Lifshitz transition, resulting in a continuous metal-insulator transition associated with a progressive change of the Fermi surface topology. In contrast to a Mott-Hubbard and Slater pictures, this spin-driven Lifshitz transition appears in systems with small electron-electron correlation and large hybridization. We show that this situation is realized in 5$d$ distorted perovskites with an half-filled $t_{2g}$ bands such as NaOsO$_3$, where the strong $p-d$ hybridization reduces the local moment, and spin-orbit coupling causes a large renormalization of the electronic mobility. This weakens the role of electronic correlations and drives the system towards an itinerant magnetic regime which enables spin-fluctuations.
Understanding the physics of strongly correlated electronic systems has been a central issue in condensed matter physics for decades. In transition metal oxides, strong correlations characteristic of narrow $d$ bands is at the origin of such remarkable properties as the Mott gap opening, enhanced effective mass, and anomalous vibronic coupling, to mention a few. SrVO$_3$, with V$^{4+}$ in a $3d^1$ electronic configuration is the simplest example of a 3D correlated metallic electronic system. Here, we focus on the observation of a (roughly) quadratic temperature dependence of the inverse electron mobility of this seemingly simple system, which is an intriguing property shared by other metallic oxides. The systematic analysis of electronic transport in SrVO$_3$ thin films discloses the limitations of the simplest picture of e-e correlations in a Fermi liquid; instead, we show that the quasi-2D topology of the Fermi surface and a strong electron-phonon coupling, contributing to dress carriers with a phonon cloud, play a pivotal role on the reported electron spectroscopic, optical, thermodynamic and transport data. The picture that emerges is not restricted to SrVO$_3$ but can be shared with other $3d$ and $4d$ metallic oxides.
We report the signatures of dynamic spin fluctuations in the layered honeycomb Li$_3$Cu$_2$SbO$_6$ compound, with a 3$d$ S = 1/2 $d^9$ Cu$^{2+}$ configuration, through muon spin rotation and relaxation ($mu$SR) and neutron scattering studies. Our zero-field (ZF) and longitudinal-field (LF)-$mu$SR results demonstrate the slowing down of the Cu$^{2+}$ spin fluctuations below 4.0 K. The saturation of the ZF relaxation rate at low temperature, together with its weak dependence on the longitudinal field between 0 and 3.2 kG, indicates the presence of dynamic spin fluctuations persisting even at 80 mK without static order. Neutron scattering study reveals the gaped magnetic excitations with three modes at 7.7, 13.5 and 33 meV. Our DFT calculations reveal that the next nearest neighbors (NNN) AFM exchange ($J_{AFM}$ = 31 meV) is stronger than the NN FM exchange ($J_{FM}$ = -21 meV) indicating the importance of the orbital degrees of freedom. Our results suggest that the physics of Li$_3$Cu$_2$SbO$_6$ can be explained by an alternating AFM chain rather than the honeycomb lattice.
Dynamical mean-field theory (DMFT) has been employed in conjunction with density functional theory (DFT+DMFT) to investigate the metal-insulator transition (MIT) of strongly correlated $3d$ electrons due to quantum confinement. We shed new light on the microscopic mechanism of the MIT and previously reported anomalous subband mass enhancement, both of which arise as a direct consequence of the quantization of V $xz(yz)$ states in the SrVO$_3$ layers. We therefore show that quantum confinement can sensitively tune the strength of electron correlations, leading the way to applying such approaches in other correlated materials.
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