Orbital-selective Mott Transition Research Articles

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.

Coupled topological flat and wide bands: Quasiparticle formation and destruction.

Flat bands amplify correlation effects and are of extensive current interest. They provide a platform to explore both topology in correlated settings and correlation physics enriched by topology. Recent experiments in correlated kagome metals have found evidence for strange-metal behavior. A major theoretical challenge is to study the effect of local Coulomb repulsion when the band topology obstructs a real-space description. In a variant to the kagome lattice, we identify an orbital-selective Mott transition in any system of coupled topological flat and wide bands. This was made possible by the construction of exponentially localized and Kramers-doublet Wannier functions, which, in turn, leads to an effective Kondo-lattice description. Our findings show how quasiparticles are formed in such coupled topological flat-wide band systems and, equally important, how they are destroyed. Our work provides a conceptual framework for the understanding of the existing and emerging strange-metal properties in kagome metals and beyond.

Antiferromagnetic fluctuations and orbital-selective Mott transition in the van der Waals ferromagnet Fe3−xGeTe2

Fe3-xGeTe2 is a layered magnetic van der Waals material of interest for both fundamental and applied research. Despite the observation of intriguing physical properties, open questions exist even on the basic features related to magnetism: is it a simple ferromagnet or are there antiferromagnetic regimes and are the moments local or itinerant. Here, we demonstrate that antiferromagnetic spin fluctuations coexist with the ferromagnetism through comprehensive elastic and inelastic neutron scattering and thermodynamic measurements. Our realistic dynamical mean-field theory calculations reveal that the competing magnetic fluctuations are driven by an orbital selective Mott transition, where only the plane-perpendicular a1g orbital of the Fe(3d) manifold remains itinerant. Our results highlight the multi-orbital character in Fe3-xGeTe2 that supports a rare coexistence of local and itinerant physics within this material.

Orbital-selective Mott and Peierls transition in HxVO2

Materials displaying metal-insulator transitions (MITs) as a function of external parameters such as temperature, pressure, or composition are most intriguing from the fundamental point of view and also hold high promise for applications. Vanadium dioxide (VO2) is one of the most prominent examples of MIT having prospective applications ranging from intelligent coatings, infrared sensing, or imaging, to Mott memory and neuromorphic devices. The key aspects conditioning possible applications are the controllability and reversibility of the transition. Here we present an intriguing MIT in hydrogenated vanadium dioxide, HxVO2. The transition relies on an increase of the electron occupancy through hydrogenation on the transition metal vanadium, driving the system insulating by a hybrid of two distinct MIT mechanisms. The insulating phase observed in HVO2 with a nominal d2 electronic configuration contrasts with other rutile d2 systems, most of which are metallic. Using spectroscopic tools and state-of-the-art many-body electronic structure calculations, our investigation reveals a correlation-enhanced Peierls and a Mott transition taking place in an orbital-selective manner cooperate to stabilize an insulating phase. The identification of the hybrid mechanism for MIT controlled by hydrogenation opens the way to radically design strategies for future correlated oxide devices by controlling phase reversibly while maintaining high crystallinity.

Eliminating Orbital Selectivity from the Metal-Insulator Transition by Strong Magnetic Fluctuations.

The orbital-selective electronic behavior is one of the most remarkable manifestations of strong electronic correlations in multiorbital systems. A prominent example is the orbital-selective Mott transition (OSMT), which is characterized by the coexistence of localized electrons in some orbitals, and itinerant electrons in other orbitals. The state-of-the-art theoretical description of the OSMT in two- and three-dimensional systems is based on local nonperturbative approximations to electronic correlations provided by dynamical mean-field theory or slave spin method. In this work we go beyond this local picture and focus on the effect of spatial collective electronic fluctuations on the OSMT. To this aim, we consider a half-filled Hubbard-Kanamori model on a cubic lattice with two orbitals that have different bandwidths. We show that strong magnetic fluctuations that are inherent in this system prevent the OSMT and favor the Néel transition that occurs at the same critical temperature for both orbitals.

Magnetism driven by strong electronic correlations in the heavily carrier-doped iron oxypnictide LaFeAsO0.49H0.51

The magnetism of the second antiferromagnetic phase (AF2) arising in the iron-based LaFeAsO$_{1-x}$H$_{x}$ superconductor for $x\gtrsim0.4$ was investigated by muon spin rotation measurements under hydrostatic pressure up to 2.6 GPa. The N\'eel temperature ($T_{\rm N}$) obtained for a sample with $x=0.51$ exhibits considerably greater sensitivity to pressure than that in the pristine antiferromagnetic phase (AF1, $x\lesssim0.06$). Moreover, while the AF1 phase is always accompanied by the structural transition (from tetragonal to orthorhombic) at a temperature ($T_{\rm s}$) which is slightly higher than $T_{\rm N}$, the AF2 phase prevails at higher pressures above $\sim$1.5 GPa where the structural transition is suppressed ($T_{\rm s}=0$). These features indicate that the microscopic origin of the AF2 phase is distinct from that of AF1, suggesting that electronic correlation plays important role in the former phase. We argue that the orbital-selective Mott transition is a plausible scenario to account for the observed pressure dependence of $T_{\rm N}$ and $T_{\rm s}$ in the AF2 phase.

Orbital differentiation in Hund metals

Orbital differentiation is a common theme in multiorbital systems, yet a complete understanding of it is still missing. Here, we consider a minimal model for orbital differentiation in Hund metals with a highly accurate method: We use the numerical renormalization group as a real-frequency impurity solver for a dynamical mean-field study of three-orbital Hubbard models, where a crystal field shifts one orbital in energy. The individual phases are characterized with dynamic correlation functions and their relation to diverse Kondo temperatures. Upon approaching the orbital-selective Mott transition, we find a strongly suppressed spin coherence scale and uncover the emergence of a singular Fermi liquid and interband doublon-holon excitations. Our theory describes the diverse polarization-driven phenomena in the $t_{2g}$ bands of materials such as ruthenates and iron-based superconductors, and our methodological advances pave the way towards real-frequency analyses of strongly correlated materials.

Hund’s metal regimes and orbital selective Mott transitions in three band systems

We analyze the electronic properties of interacting crystal field split three band systems. Using a rotationally invariant slave boson approach we analyze the behavior of the electronic mass renormalization as a function of the intralevel repulsion U, the Hund’s coupling J, the crystal field splitting, and the number of electrons per site n. We first focus on the case in which two of the bands are identical and the levels of the third one are shifted by with respect to the former. We find an increasing quasiparticle mass differentiation between the bands, for system away from half-filling (n = 3), as the Hubbard interaction U is increased. This leads to orbital selective Mott transitions where either the higher energy band (for 4 > n > 3) or the lower energy degenerate bands (2 < n < 3) become insulating for U larger than a critical interaction . Away from the half-filled case there is a wide range of parameters for where the system presents a Hund’s metal phase with the physics dominated by the local high spin multiplets. Finally, we study the fate of the n = 2 Hund’s metal as the energy splitting between orbitals is increased for different possible crystal distortions. We find a strong sensitivity of the Hund’s metal regime to crystal fields due to the opposing effects of J and the crystal field splittings on the charge distribution between the bands.

Cooperative effects of strain and electron correlation in epitaxial VO2 and NbO2

We investigate the electronic structure of epitaxial VO2 films in the rutile phase using density functional theory combined with the slave-spin method (DFT + SS). In DFT + SS, multi-orbital Hubbard interactions are added to a DFT-fit tight-binding model, and slave spins are used to treat electron correlations. We find that while stretching the system along the rutile c-axis results in a band structure favoring anisotropic orbital fillings, electron correlations favor equal filling of the t2g orbitals. These two distinct effects cooperatively induce an orbital-dependent redistribution of the electron occupations and spectral weights, driving strained VO2 toward an orbital selective Mott transition (OSMT). The simulated single-particle spectral functions are directly compared to V L-edge resonant X-ray photoemission spectroscopy of epitaxial 10 nm VO2/TiO2 (001) and (100) strain orientations. Excellent agreement is observed between the simulations and experimental data regarding the strain-induced evolution of the lower Hubbard band. Simulations of rutile NbO2 under similar strain conditions are performed, and we predict that an OSMT will not occur in rutile NbO2. Our prediction is supported by the high-temperature hard x-ray photoelectron spectroscopy measurement on relaxed NbO2 (110) thin films with no trace of the lower Hubbard band. Our results indicate that electron correlations in VO2 are important and can be modulated even in the rutile phase before the Peierls instability sets in.

Microscopic description of localization-delocalization transitions in BaFe2S3

Unusual metallic states involving breakdown of the standard Fermi-liquid picture of long-lived quasiparticles in well-defined band states emerge at low temperatures near correlation-driven Mott transitions. Prominent examples are ill-understood metallic states in $d$- and $f$-band compounds near Mott-like transitions. Finding of superconductivity in solid O$_{2}$ on the border of an insulator-metal transition at high pressures close to 96~GPa is thus truly remarkable. Neither the insulator-metal transition nor superconductivity are understood satisfactorily. Here, we undertake a first step in this direction by focussing on the pressure-driven insulator-metal transition using a combination of first-principles density-functional and many-body calculations. We report a striking result: the finding of an orbital-selective Mott transition in a pure $p$-band elemental system. We apply our theory to understand extant structural and transport data across the transition, and make a specific two-fluid prediction that is open to future test. Based thereupon, we propose a novel scenario where soft multiband modes built from microscopically coexisting itinerant and localized electronic states are natural candidates for the pairing glue in pressurized O$_{2}$.

Orbital Origin of Extremely Anisotropic Superconducting Gap in Nematic Phase of FeSe Superconductor

The iron-based superconductors are characterized by multiple-orbital physics where all the five Fe 3$d$ orbitals get involved. The multiple-orbital nature gives rise to various novel phenomena like orbital-selective Mott transition, nematicity and orbital fluctuation that provide a new route for realizing superconductivity. The complexity of multiple-orbital also asks to disentangle the relationship between orbital, spin and nematicity, and to identify dominant orbital ingredients that dictate superconductivity. The bulk FeSe superconductor provides an ideal platform to address these issues because of its simple crystal structure and unique coexistence of superconductivity and nematicity. However, the orbital nature of the low energy electronic excitations and its relation to the superconducting gap remain controversial. Here we report direct observation of highly anisotropic Fermi surface and extremely anisotropic superconducting gap in the nematic state of FeSe superconductor by high resolution laser-based angle-resolved photoemission measurements. We find that the low energy excitations of the entire hole pocket at the Brillouin zone center are dominated by the single $d_{xz}$ orbital. The superconducting gap exhibits an anti-correlation relation with the $d_{xz}$ spectral weight near the Fermi level, i.e., the gap size minimum (maximum) corresponds to the maximum (minimum) of the $d_{xz}$ spectral weight along the Fermi surface. These observations provide new insights in understanding the orbital origin of the extremely anisotropic superconducting gap in FeSe superconductor and the relation between nematicity and superconductivity in the iron-based superconductors.

Correlation-driven Lifshitz transition and orbital order in a two-band Hubbard model

We study by dynamical mean field theory the ground state of a quarter-filled Hubbard model of two bands with different bandwidths. At half-filling, this model is known to display an orbital selective Mott transition, with the narrower band undergoing Mott localisation while the wider one being still itinerant. At quarter-filling, the physical behaviour is different and to some extent reversed. The interaction generates an effective crystal field splitting, absent in the Hamiltonian, that tends to empty the narrower band in favour of the wider one, which also become more correlated than the former at odds with the orbital selective paradigm. Upon increasing the interaction, the depletion of the narrower band can continue till it empties completely and the system undergoes a topological Lifshitz transition into a half-filled single-band metal that eventually turns insulating. Alternatively, when the two bandwidths are not too different, a first order Mott transition intervenes before the Lifshitz's one. The properties of the Mott insulator are significantly affected by the interplay between spin and orbital degrees of freedom.

Dynamic signature of orbital selective Mott transition in the metallic phase of VO2

An orbital-selective technique, nuclear magnetic resonance (NMR) spectroscopy, which could simultaneously probe the atomic structure and electronic properties, was employed to address the ‘bad metal’ behaviors, i.e., negligible electron thermal conductivity in the metallic phase of VO2. The measured electric field gradients at V sites by 51V NMR were found to evolve significantly in the pure metallic phase within the vicinity of structural phase transition temperatures, unexpected in a simple metal within this temperature region according to structural analysis by diffraction. This abnormal temperature-dependent local symmetry evolution can be well explained by a simple phenomenological model of orbital selective Mott transition in this multiorbital system.

Spectroscopic Studies on the Metal-Insulator Transition Mechanism in Correlated Materials.

The metal-insulator transition (MIT) in correlated materials is a novel phenomenon that accompanies a large change in resistivity, often many orders of magnitude. It is important in its own right but its switching behavior in resistivity can be useful for device applications. From the material physics point of view, the starting point of the research on the MIT should be to understand the microscopic mechanism. Here, an overview of recent efforts to unravel the microscopic mechanisms for various types of MITs in correlated materials is provided. Research has focused on transition metal oxides (TMOs), but transition metal chalcogenides have also been studied. Along the way, a new class of MIT materials is discovered, the so-called relativistic Mott insulators in 5d TMOs. Distortions in the MO6 (M = transition metal) octahedron are found to have a large and peculiar effect on the band structure in an orbital dependent way, possibly paving a way to the orbital selective Mott transition. In the final section, the character of the materials suitable for applications is summarized, followed by a brief discussion of some of the efforts to control MITs in correlated materials, including a dynamical approach using light.

A dynamical mean-field study of orbital-selective Mott phase enhanced by next-nearest neighbor hopping

The dynamical mean-field theory is employed to study the orbital-selective Mott transition (OSMT) of the two-orbital Hubbard model with nearest neighbor hopping and next-nearest neighbor (NNN) hopping. The NNN hopping breaks the particle-hole symmetry at half filling and gives rise to an asymmetric density of states (DOS). Our calculations show that the broken symmetry of DOS benefits the OSMT, where the region of the orbital-selective Mott phase significantly extends with the increasing NNN hopping integral. We also find that Hund's rule coupling promotes OSMT by blocking the orbital fluctuations, but the influence of NNN hopping is more remarkable.

Dynamic signature of orbital selective Mott transition in the metallic phase of VO2

Dynamic signature of orbital selective Mott transition in the metallic phase of VO2

Distinct nature of orbital-selective Mott phases dominated by low-energy local spin fluctuations

Quantum orbital selective Mott (OSM) transitions are investigated within dynamical mean-field theory based on a two-orbital Hubbard model with different bandwidth at half filling. We find two distinct OSM phases both showing coexistence of itinerant electrons and localized spins, dependent on whether the Hund's coupling is full or of Ising type. The critical values and the nature of the OSM transitions are efficiently determined by entanglement entropy. We reveal that vanishing of the Kondo energy scale evidenced by absence of local spin fluctuations at low frequency in local dynamical spin susceptibility is responsible for the appearance of non-Fermi-liquid OSM phase in Ising Hund's coupling case. We argue that this scenario can also be applied to account for emergent quantum non-Fermi liquid in one-band Hubbard model when short-range antiferromagnetic order is considered.

Orbital physics in transition metal compounds: new trends

The present review discusses different effects related to orbital degrees of freedom. Leaving aside such aspects as the superexchange mechanism of cooperative Jahn–Teller distortions and various properties of ‘Kugel–Khomskii’-like models, we mostly concentrate on other phenomena, which are the focus of modern condensed matter physics. After a general introduction, we start with a discussion of the concept of effective reduction of dimensionality due to orbital degrees of freedom and consider such phenomena as the orbitally driven Peierls effect and the formation of small clusters of ions in the vicinity of the Mott transition, which behave like ‘molecules’ embedded in a solid. The second large part is devoted to orbital-selective effects, such as the orbital-selective Mott transition and the suppression of magnetism due to the fact that the electrons on some orbitals start to form singlet molecular orbitals. At the end, the rapidly growing field of so-called ‘spin–orbit-dominated’ transition metal compounds is briefly reviewed, including such topics as the interplay between the spin–orbit coupling and the Jahn–Teller effect, the formation of the spin–orbit driven Mott and Peierls states, the role of orbital degrees of freedom in generating the Kitaev exchange coupling, and the singlet (excitonic) magnetism in 4d and 5d transition metal compounds.

Spin-selective thermalization plateau in the mass-imbalanced Hubbard model

We use time-dependent non-equilibrium dynamical mean-field theory with weak-coupling auxiliary-field continuous time quantum Monte Carlo as an impurity solver to study the thermalization behavior of the mass-imbalanced single-band Hubbard model after a quench of the Coulomb interaction from the non-interacting limit to a finite positive value. By contrast, when the Coulomb interaction in our model is increased under equilibrium conditions, the quasi-particle weight for spin-up and spin-down (the mass imbalance) electrons approach zero simultaneously, indicating the absence of an orbital selective Mott transition. Our out-of-equilibrium study suggests that there exists a time window where an orbital selective dynamical phase transition occurs. The dynamical phase transition is characterized by the relaxation behavior of energy (kinetic and Coulomb interaction) and the spin-resolved momentum-dependent occupation. To make connection with possible experiments, we calculate the spin-resolved two-time optical conductivity, which confirms the orbital-selective thermalization plateau. We find the time window for the orbital selective dynamical phase transition grows as the mass imbalance increases.

Analytical slave-spin mean-field approach to orbital selective Mott insulators

We use the slave-spin mean-field approach to study particle-hole symmetric one- and two-band Hubbard models in presence of Hund's coupling interaction. By analytical analysis of Hamiltonian, we show that the locking of the two orbitals vs.\,orbital-selective Mott transition can be formulated within a Landau-Ginzburg framework. By applying the slave-spin mean-field to impurity problem, we are able to make a correspondence between impurity and lattice. We also consider the stability of the orbital selective Mott phase to the hybridization between the orbitals and study the limitations of the slave-spin method for treating inter-orbital tunnellings in the case of multi-orbital Bethe lattices with particle-hole symmetry.