Orbital-selective Mott Phase Research Articles

Kondo breakdown in multi-orbital Anderson lattices induced by destructive hybridization interference

In this paper we consider a multi-band extension to the periodic Anderson model. We use a single site DMFT(NRG) in order to study the impact of the conduction band mediated effective hopping of the correlated electrons between the correlated orbitals onto the heavy Fermi-liquid formation. Whereas the hybridization of a single impurity model with two distinct conduction bands always adds up constructively, T_{K}\propto \exp(-\mathrm{const}\, U/(\Gamma_1+\Gamma_2))TK∝exp(−constU/(Γ1+Γ2)), we show that this does not have to be the case in lattice models, where, in remarkable contrast, also an low-energy Fermi-liquid scale T_0\propto \exp(-\mathrm{const}\, U/(\Gamma_1-\Gamma_2))T0∝exp(−constU/(Γ1−Γ2)) can emerge due to quantum interference effects in multi-band models, where UU denotes the local Coulomb matrix element of the correlated orbitals and \Gamma_iΓi the local hybridization strength of band ii. At high symmetry points, heavy Fermi-liquid formation is suppressed which is associated with a breakdown of the Kondo effect. This results in an asymptotically scale-invariant (i.e., power-law) spectrum of the correlated orbitals \propto|\omega|^{1/3}∝|ω|1/3, indicating non-Fermi liquid properties of the quantum critical point, and a small Fermi surface including only the light quasi-particles. This orbital selective Mott phase demonstrates the possibility of metallic local criticality within the general framework of ordinary single site DMFT.

Quantitative determination of the orbital-selective Mott transition and quantum entanglement in the orbital-selective Mott phase

Quantitative determination of the orbital-selective Mott transition and quantum entanglement in the orbital-selective Mott phase

Orbital-Selective Mott Transition Effects and Nontrivial Topology of Iron Chalcogenide.

The iron-based superconductor FeSe_{1-x}Te_{x} has recently gained significant attention as a host of two distinct physical phenomena: (i)Majorana zero modes that can serve as potential topologically protected qubits, and (ii)a realization of the orbital-selective Mott transition. In this Letter, we connect these two phenomena and provide new insights into the interplay between strong electronic correlations and nontrivial topology in FeSe_{1-x}Te_{x}. Using linearized quasiparticle self-consistent GW plus dynamical mean-field theory, we show that the topologically protected Dirac surface state has substantial Fe(d_{xy}) character. The proximity to the orbital-selective Mott transition plays a dual role: it facilitates the appearance of the topological surface state by bringing the Dirac cone close to the chemical potential but destroys the Z_{2} topological superconductivity when the system is too close to the orbital-selective Mott phase. We derive a reduced effective Hamiltonian that describes the topological band. Its parameters capture all the chemical trends found in the first principles calculation. Our findings provide a framework for further study of the interplay between strong electronic correlations and nontrivial topology in other iron-based superconductors.

Orbital-Selectivity-Induced Robust Quantum Anomalous Hall Effect in Hund's Metals MgFeP.

Ferromagnetic (FM) states with high Curie temperatures (Tc) and strong spin-orbit coupling (SOC) are indispensable for the long-sought room-temperature quantum anomalous Hall (QAH) effects. Here, we propose a two-dimensional (2D) iron-based monolayer MgFeP that exhibits a notably high FM Tc (about 1525 K) along with exceptional structural stabilities. The unique multiorbital nature in MgFeP, where localized and dxz/yz orbitals coexist with itinerant dxy and dz2 orbitals, renders the monolayer a Hund's metal and in an orbital-selective Mott phase (OSMP). This OSMP triggers an FM double exchange mechanism, rationalizing the high Tc in the Hund's metal. This material transitions to a QAH insulator upon consideration of the SOC effect. By leveraging orbital selectivity, the QAH band gap can be enlarged by more than two times (to 137 meV). Our findings showcase Hund's metals as a promising material platform for realizing high-performance quantum topological electronic devices.

Stability of the interorbital-hopping mechanism for ferromagnetism in multi-orbital Hubbard models

The emergence of insulating ferromagnetic phase in iron oxychalcogenide chain system has been recently argued to be originated by interorbital hopping mechanism. However, the practical conditions for the stability of such mechanism still prevents the observation of ferromagnetic in many materials. Here, we study the stability range of such ferromagnetic phase under modifications in the crystal fields and electronic correlation strength, constructing a theoretical phase diagram. We find a rich emergence of phases, including a ferromagnetic Mott insulator, a ferromagnetic orbital-selective Mott phase, together with antiferromagnetic and ferromagnetic metallic states. We characterize the stability of the ferromagnetic regime in both the Mott insulator and the ferromagnetic orbital-selective Mott phase forms. We identify a large stability range in the phase diagram at both intermediate and strong electronic correlations, demonstrating the capability of the interorbital hopping mechanism in stabilizing ferromagnetic insulators. Our results may enable additional design strategies to expand the relatively small family of known ferromagnetic insulators.

Signatures of orbital selective Mott state in doped Sr3Ru2O7

Bilayer Strontium Ruthenate ${\mathrm{Sr}}_{3}{\mathrm{Ru}}_{2}{\mathrm{O}}_{7}$ is a strongly correlated electronic system that shows diverse electronic and structural phases. Upon doping with Mn, an orbital selective Mott phase is observed before the material transitions to a Mott insulating state. Additionally, Mn doping leads to the emergence of an antiferromagnetic state with ${\mathbit{q}}_{\mathbit{AFM}}=(\ensuremath{\pi}/2,\ensuremath{\pi}/2)$ ordering wave vector. Quasiparticle interference (QPI) experiments find a sharp but highly dispersive peak at the AFM wave vector. Another set of QPI peaks is observed at ${\mathbit{q}}^{*}=(\ensuremath{\pi},0),$ possibly due to a charge order effect. In this work we utilize a tight binding model relevant to Mn doped ${\mathrm{Sr}}_{3}{\mathrm{Ru}}_{2}{\mathrm{O}}_{7}$, and show that the origin of observed orbital selective Mott phase is inherently dependent upon the presence of a strong onsite exchange interaction and oxygen octahedral rotation suppression induced by the Mn doping. We further find that the experimentally observed QPI spectra, including the peaks at ${\mathbit{q}}_{\mathbit{AFM}}$, and ${\mathbit{q}}^{*}$ wave vectors can be concomitantly explained within this formalism.

Is the Orbital-Selective Mott Phase Stable against Interorbital Hopping?

The localization-delocalization transition is at the heart of strong correlation physics. Recently, there is great interest in multiorbital systems where this transition can be restricted to certain orbitals, leading to an orbital-selective Mott phase (OSMP). Theoretically, the OSMP is widely studied for kinetically decoupled orbitals, but the effect of interorbital hopping remains unclear. Here, we show how nonlocal interorbital hopping leads to local hybridization in single-site dynamical mean-field theory (DMFT). Under fairly general circumstances, this implies that, at zero temperature, the OSMP, involving the Mott-insulating state of one orbital, is unstable against interorbital hopping to a different, metallic orbital. We further show that the coherence scale below which all electrons are itinerant is very small and gets exponentially suppressed even if the interorbital hopping is not overly small. Within this framework, the OSMP with interorbital hopping may thus reach down to extremely low temperatures T, but not to T=0. Accordingly, it is part of a coherence-incoherence crossover and not a quantum critical point. We present analytical arguments supported by numerical results using the numerical renormalization group as a DMFT impurity solver. We also compare our findings with previous slave-spin studies.

Signature of Kondo hybridisation with an orbital-selective Mott phase in 4d Ca2−xSrxRuO4

AbstractThe heavy fermion state with Kondo-hybridisation (KH), usually manifested in f-electron systems with lanthanide or actinide elements, was recently discovered in several 3d transition metal compounds without f-electrons. However, KH has not yet been observed in 4d/5d transition metal compounds, since more extended 4d/5d orbitals do not usually form flat bands that supply localised electrons appropriate for Kondo pairing. Here, we report a substitution- and temperature-dependent angle-resolved photoemission study on 4d Ca2−xSrxRuO4, which shows the signature of KH. We observed a spectral weight transfer in the γ-band, reminiscent of an orbital-selective Mott phase (OSMP). The Mott localised γ-band induces the KH with an itinerant β-band, resulting in spectral weight suppression around the Fermi level. Our work demonstrates the evolution of the OSMP with possible KH among 4d electrons, and thereby expands the material boundary of Kondo physics to 4d multi-orbital systems.

Correlation-driven electronic reconstruction in FeTe1\u2212xSex

Electronic correlation is of fundamental importance to high temperature superconductivity. While the low energy electronic states in cuprates are dominantly affected by correlation effects across the phase diagram, observation of correlation-driven changes in fermiology amongst the iron-based superconductors remains rare. Here we present experimental evidence for a correlation-driven reconstruction of the Fermi surface tuned independently by two orthogonal axes of temperature and Se/Te ratio in the iron chalcogenide family FeTe1−xSex. We demonstrate that this reconstruction is driven by the de-hybridization of a strongly renormalized dxy orbital with the remaining itinerant iron 3d orbitals in the emergence of an orbital-selective Mott phase. Our observations are further supported by our theoretical calculations to be salient spectroscopic signatures of such a non-thermal evolution from a strongly correlated metallic phase into an orbital-selective Mott phase in dxy as Se concentration is reduced.

Orbital-selective Mott phase and non-Fermi liquid in FePS3

The layered metal phosphorous trisulfide FePS$_3$ is reported to be a Mott insulator at ambient conditions and to undergo structural and insulator-metal phase transitions under pressure. However, the character of the resulting metallic states has not been understood clearly so far. Here, we theoretically study the phase transitions of FePS$_3$ using first-principles methods based on density functional theory and embedded dynamical mean field theory. We find that the Mott transition in FePS$_3$ can be orbital-selective, with $t_{2g}$ states undergoing a correlation-induced insulator-to-metal transition while $e_g$ states remain gapped. We show that this orbital-selective Mott phase, which occurs only when non-hydrostatic pressure is used, is a bad metal (or non-Fermi liquid) with large fluctuating moments due to Hund's coupling. Further application of pressure increases the crystal-field splitting and converts the system to a conventional Fermi liquid with low-spin configurations dominant. Our results show that FePS$_3$ is a novel example of a system that realizes an orbital-selective Mott phase, allowing tuning between correlated and uncorrelated metallic properties in an accessible pressure range ($\leq$ 18 GPa).

Magnetic states of the quasi-one-dimensional iron chalcogenide Ba2FeS3

Quasi-one-dimensional iron-based ladders and chains, with the $3d$ iron electronic density $n=6$, are attracting considerable attention. Recently, a new iron chain system ${\mathrm{Ba}}_{2}{\mathrm{FeS}}_{3}$, also with $n=6$, was prepared under high-pressure and high-temperature conditions. Here the magnetic and electronic phase diagrams are theoretically studied for this quasi-one-dimensional compound. Based on first-principles calculations, a strongly anisotropic one-dimensional electronic band behavior near the Fermi level was observed. In addition, a three-orbital electronic Hubbard model for this chain was constructed. Introducing the Hubbard and Hund couplings and studying the model via the density matrix renormalization group (DMRG) method, we studied the ground-state phase diagram. A robust staggered $\ensuremath{\uparrow}\text{\ensuremath{-}}\ensuremath{\downarrow}\text{\ensuremath{-}}\ensuremath{\uparrow}\text{\ensuremath{-}}\ensuremath{\downarrow}$ AFM region was unveiled in the chain direction, consistent with our density functional theory (DFT) calculations. Furthermore, at intermediate Hubbard $U$ coupling strengths, this system was found to display an orbital selective Mott phase (OSMP) with one localized orbital and two itinerant metallic orbitals. At very large $U/W$ $(W=\mathrm{bandwidth})$, the system displays Mott insulator characteristics, with two orbitals half-filled and one doubly occupied. Our results for high pressure ${\mathrm{Ba}}_{2}{\mathrm{FeS}}_{3}$ provide guidance to experimentalists and theorists working on this one-dimensional iron chalcogenide chain material.

Orbital-selective Peierls phase in the metallic dimerized chain MoOCl2

Using ab initio density functional theory, here we systematically study the monolayer ${\mathrm{MoOCl}}_{2}$ with a $4{d}^{2}$ electronic configuration. Our main result is that an orbital-selective Peierls phase (OSPP) develops in ${\mathrm{MoOCl}}_{2}$, resulting in the dimerization of the Mo chain along the $b$ axis. Specifically, the Mo-${d}_{xy}$ orbitals form robust molecular-orbital states inducing localized ${d}_{xy}$ singlet dimers, while the Mo-${d}_{xz/yz}$ orbitals remain delocalized and itinerant. Our study shows that ${\mathrm{MoOCl}}_{2}$ is globally metallic, with the Mo-${d}_{xy}$ orbital bonding-antibonding splittings opening a gap and the Mo-${d}_{xz/yz}$ orbitals contributing to the metallic conductivity. Overall, the results resemble the recently much discussed orbital-selective Mott phase but with the localized band induced by a Peierls distortion instead of Hubbard interactions. Finally, we also qualitatively discuss the possibility of OSPP in the $3{d}^{2}$ configuration, as in ${\mathrm{CrOCl}}_{2}$.

Quantum magnetism of iron-based ladders: Blocks, spirals, and spin flux

Motivated by increasing experimental evidence of exotic magnetism in low-dimensional iron-based materials, we present a comprehensive theoretical analysis of magnetic states of the multiorbital Hubbard ladder in the orbital-selective Mott phase (OSMP). The model we used is relevant for iron-based compounds of the AFe$_2$X$_3$ family (where A${}={}$Cs, Rb, Ba, K are alkali metals and X${}={}$S, Se are chalcogenides). To reduce computational effort, and obtain almost exact numerical results in the ladder geometry, we utilize a low-energy description of the Hubbard model in the OSMP - the generalized Kondo-Heisenberg Hamiltonian. Our main result is the doping vs interaction magnetic phase diagram. We reproduce the experimental findings on the AFe$_2$X$_3$ materials, especially the exotic block magnetism of BaFe$_2$Se$_3$ (antiferromagnetically coupled $2\times 2$ ferromagnetic islands of the $\uparrow\uparrow\downarrow\downarrow$ form). As in recent studies of the chain geometry, we also unveil block magnetism beyond the $2 \times 2$ pattern (with block sizes varying as a function of the electron doping) and also an interaction-induced frustrated block-spiral state (a spiral order of rigidly rotating ferromagnetic islands). Moreover, we predict new phases beyond the one-dimensional system: a robust regime of phase separation close to half-filling, incommensurate antiferromagnetism for weak interaction, and a quantum spin-flux phase of staggered plaquette spin currents at intermediate doping. Finally, exploiting the bonding/antibonding band occupations, we provide an intuitive physical picture giving insight into the structure of the phase diagram.

Electronic correlation-driven orbital polarization transitions in the orbital-selective Mott compound Ba2CuO4−δ

The electronic states near the Fermi level of recently discovered superconductor ${\mathrm{Ba}}_{2}{\mathrm{CuO}}_{4\ensuremath{-}\ensuremath{\delta}}$ consist primarily of the Cu ${d}_{{x}^{2}\ensuremath{-}{y}^{2}}$ and ${d}_{3{z}^{2}\ensuremath{-}{r}^{2}}$ orbitals. We investigate the electronic correlation effect and the orbital polarization of an effective two-orbital Hubbard model mimicking the low-energy physics of ${\mathrm{Ba}}_{2}{\mathrm{CuO}}_{4\ensuremath{-}\ensuremath{\delta}}$ in the hole-rich regime by utilizing the dynamical mean-field theory with the Lanczos method as the impurity solver. We find that the hole-overdoped ${\mathrm{Ba}}_{2}{\mathrm{CuO}}_{4\ensuremath{-}\ensuremath{\delta}}$ with $3{d}^{8}$ (${\mathrm{Cu}}^{3+}$) is in the orbital-selective Mott phase (OSMP) at half-filling, and the typical two-orbital feature remains in ${\mathrm{Ba}}_{2}{\mathrm{CuO}}_{4\ensuremath{-}\ensuremath{\delta}}$ when the electron filling approaches ${n}_{e}\ensuremath{\sim}2.5$, which closely approximates to the experimental hole doping for the emergence of the high-${T}_{c}$ superconductivity. We also obtain that the orbital polarization is very stable in the OSMP, and the multiorbital correlation can drive orbital polarization transitions. These results indicate that in hole-overdoped ${\mathrm{Ba}}_{2}{\mathrm{CuO}}_{4\ensuremath{-}\ensuremath{\delta}}$ the OSMP physics and orbital polarization, local magnetic moment, and spin or orbital fluctuations still exist. We propose that our present results are also applicable to ${\mathrm{Sr}}_{2}{\mathrm{CuO}}_{4\ensuremath{-}\ensuremath{\delta}}$ and other two-orbital cuprates, demanding an unconventional multiorbital superconducting scenario in hole-overdoped high-${T}_{c}$ cuprates.

Orbital-selective coherence-incoherence crossover and metal-insulator transition in Cu-doped NaFeAs

We study the effects of electron-electron interactions and hole doping on the electronic structure of Cu-doped NaFeAs using the density functional theory plus dynamical mean-field theory (DFT+DMFT) method. In particular, we employ an effective multi-orbital Hubbard model with a realistic bandstructure of NaFeAs in which Cu-doping was modeled within a rigid band approximation and compute the evolution of the spectral properties, orbital-dependent electronic mass renormalizations, and magnetic properties of NaFeAs upon doping with Cu. In addition, we perform fully charge self-consistent DFT+DMFT calculations for the long-range antiferromagnetically ordered Na(Fe,Cu)As with Cu $x=0.5$ with a real-space ordering of Fe and Cu ions. Our results reveal a crucial importance of strong electron-electron correlations and local potential difference between the Cu and Fe ions for understanding the \textbf{k}-resolved spectra of Na(Fe,Cu)As. Upon Cu-doping, we observe a strong orbital-dependent localization of the Fe $3d$ states accompanied by a large renormalization of the Fe $xy$ and $xz$/$yz$ orbitals. Na(Fe,Cu)As exhibits bad metal behavior associated with a coherence-to-incoherence crossover of the Fe $3d$ electronic states and local moments formation near a Mott metal-insulator transition (MIT). For heavily doped NaFeAs with Cu $x \sim 0.5$ we obtain a Mott insulator with a band gap of $\sim$0.3 eV characterized by divergence of the quasiparticle effective mass of the Fe $xy$ states. In contrast to this, the quasiparticle weights of the Fe $xz$/$yz$ and $e_g$ states remain finite at the MIT. The MIT occurs via an orbital-selective Mott phase to appear at Cu $x\simeq0.375$ with the Fe $xy$ states being Mott localized. We propose the possible importance of Fe/Cu disorder to explain the magnetic properties of Cu-doped NaFeAs.

Block–spiral magnetism: An exotic type of frustrated order

Competing interactions in quantum materials induce exotic states of matter such as frustrated magnets, an extensive field of research from both the theoretical and experimental perspectives. Here, we show that competing energy scales present in the low-dimensional orbital-selective Mott phase (OSMP) induce an exotic magnetic order, never reported before. Earlier neutron-scattering experiments on iron-based 123 ladder materials, where OSMP is relevant, already confirmed our previous theoretical prediction of block magnetism (magnetic order of the form [Formula: see text]). Now we argue that another phase can be stabilized in multiorbital Hubbard models, the block-spiral state. In this state, the magnetic islands form a spiral propagating through the chain but with the blocks maintaining their identity, namely rigidly rotating. The block-spiral state is stabilized without any apparent frustration, the common avenue to generate spiral arrangements in multiferroics. By examining the behavior of the electronic degrees of freedom, parity-breaking quasiparticles are revealed. Finally, a simple phenomenological model that accurately captures the macroscopic spin spiral arrangement is also introduced, and fingerprints for the neutron-scattering experimental detection are provided.

Anisotropic transport properties of tetragonal SrFeO2.84 single crystal

The tetragonal SrFeO2.84 single crystal was grown by using floating zone method, and followed by resistivity and magnetization measurements with respect to temperature. Here, the magnetization data shows an antiferromagnetic ordering below 63 K, accompanied by the formation of the charge ordering. However, an anomalous insulator to metal transition occurs below 40 K in the basal plane of SrFeO2.84 single crystal, while the resistivity along the c axis still keeps insulating. Our results reveal that, the anisotropy of resistivity in SrFeO2.84 is caused by the magnetically driven orbital-selective Mott phase transition.

Doublon-holon excitations split by Hund's rule coupling within the orbital-selective Mott phase

Multiorbital interactions have the capacity to produce an interesting kind of doublon-holon bound state that consists of a single-hole state in one band and a doubly-occupied state in another band. Interband doublon-holon pair excitations in the two-orbital Hubbard model are studied by using dynamical mean-field theory with the Lanczos method as the impurity solver. We find that the interband bound states may provide several in-gap quasiparticle peaks in the density of states of the narrow band in the orbital-selective Mott phase with a small Hund's rule coupling ($J$). There exists a corresponding energy relation between the in-gap states of the narrow band and the peaks in the excitation spectrum of the doublon for the wide band. We also find that the spin flip and pair-hopping Hund interactions can divide one quasiparticle peak into two peaks, where the splitting energy increases linearly with increasing $J$. Strong Hund's rule coupling can move the interband doublon-holon pair excitations outside the Mott gap and restrict the bound states by suppressing the orbital selectivity of the doubly-occupied and single-hole states.

Novel Magnetic Block States in Low-Dimensional Iron-Based Superconductors.

Inelastic neutron scattering recently confirmed the theoretical prediction of a ↑↑↓↓-magnetic state along the legs of quasi-one-dimensional iron-based ladders in the orbital-selective Mott phase (OSMP). We show here that electron doping of the OSMP induces a whole class of novel block states with a variety of periodicities beyond the previously reported π/2 pattern. We discuss the magnetic phase diagram of the OSMP regime that could be tested by neutrons once appropriate quasi-1D quantum materials with the appropriate dopings are identified.

Fingerprints of an orbital-selective Mott phase in the block magnetic state of BaFe2Se3 ladders

Resonant Inelastic X-Ray Scattering (RIXS) experiments on the iron-based ladder BaFe2Se3 unveiled an unexpected two-peak structure associated with local orbital (dd) excitations in a block-type antiferromagnetic phase. A mixed character between correlated band-like and localized excitations was also reported. Here, we use the density matrix renormalization group method to calculate the momentum-resolved charge- and orbital-dynamical response functions of a multi-orbital Hubbard chain. Remarkably, our results qualitatively resemble the BaFe2Se3 RIXS data, while also capturing the presence of long-range magnetic order as found in neutron scattering, only when the model is in an exotic orbital-selective Mott phase (OSMP). In the calculations, the experimentally observed zero-momentum transfer RIXS peaks correspond to excitations between itinerant and Mott insulating orbitals. We provide experimentally testable predictions for the momentum-resolved charge and orbital dynamical structures, which can provide further insight into the OSMP regime of BaFe2Se3.