Mott State Research Articles

Realizing multiorbital Hubbard model with commensurate fillings in the paramagnetic phase of triangular magnets (X = Mn, Co, Ni)

The multiorbital Hubbard model is renowned for its rich phase diagram, characterized by various filling-dependent Mott transitions. However, controlling electron filling to explore the complete phase diagram within a single material remains challenging. In this study, we investigate three members of a correlated magnet family: Na2BaX(PO4)2 (where X = Mn, Co, Ni). Our focus is on revealing their unusual electronic structure related to the different electron fillings. Despite differences in their effective angular momentum, our first-principles calculations reveal a strikingly similar flat-band electronic structure across all three systems. Remarkably, we found that their distinct valence configurations lead to a similar response to electronic correlations in the high-temperature paramagnetic phases, which nicely realizes Mott states with different electron concentrations. Thus, these systems can be conceptualized as multiorbital Hubbard models with differing electron fillings. Our work unifies the understanding of these structurally similar systems and opens new avenues for exploring correlated electronic structures with distinct fillings.

Phases and coherence of strongly interacting finite bosonic systems in shallow optical lattice

We explore the ground states of strongly interacting bosons in the vanishingly small and weak lattices using the multiconfiguration time-dependent Hartree method for bosons (MCTDHB) which calculate numerically exact many-body wave function. Two new many-body phases: fragmented or quasi superfluid (QSF) and incomplete fragmented Mott or quasi Mott insulator (QMI) are emerged due to the strong interplay between short-range contact interaction and lattice depth. Fragmentation is utilized as a figure of merit to distinguish these two new phases. We utilize the eigenvalues of the reduced one-body density matrix and define an order parameter that characterizes the pathway from a very weak lattice to a deep lattice. We provide a detailed investigation through the measures of one- and two-body correlations and information entropy. We find that the structures in one- and two-body coherence are good markers to understand the gradual built-up of intra-well correlation and decay of inter-well correlation with increase in lattice depth. For the dipolar interaction, the many-body features become more distinct and true Mott state can appear even in a shallow lattice. Whereas, for incommensurate fraction of particles, incomplete localization happens that exhibits distinct features in the measure of two-body coherence.

Tunable 5d-t2g Mott State and Monoatomic Layer Two-Dimensional Electron Gas Realized in Spin–Orbit-Coupled SrIrO3 through Heterostructuring

Tunable 5d-t_2g Mott State and Monoatomic Layer Two-Dimensional Electron Gas Realized in Spin–Orbit-Coupled SrIrO₃ through Heterostructuring

Can Orbital-Selective Néel Transitions Survive Strong Nonlocal Electronic Correlations?

Spin- or orbital-selective behaviors in correlated electron materials offer rich promise for spintronics or orbitronics phenomena and applications deriving from them. Strong local electronic Coulomb correlations might lead to an orbital-selective Mott state, characterized by the coexistence of localized electrons in some orbitals with itinerant electrons in others. Nonlocal electronic fluctuations are much more entangled in orbital space than the local ones. For this reason, finding orbital-selective phenomena related to nonlocal correlations, such as orbital-selective magnetic transitions, is a challenge. In this Letter, we investigate possibilities to realize an orbital-selective Néel transition (OSNT). We illustrate that stabilizing this state requires a decoupling of magnetic fluctuations in different orbitals, which can only be realized in the absence of Hund's exchange coupling. On the basis of two-orbital calculations for a Hubbard model with different bandwidths we show that the proposed OSNT can be found all the way from the weak to the strong coupling regime. In the weak coupling regime the transition is governed by a Slater mechanism and thus occurs first for the narrow orbital. At strong coupling a Heisenberg mechanism of the OSNT sets in, and the transition occurs first for the wide orbital. Remarkably, at intermediate values of the interaction we find a nontrivial regime of the OSNT, where the Slater mechanism leads to a Néel transition occurring first for the wide orbital. Our work suggests strategies for searching for orbital-selective Néel ordering in real materials in view of possible spin-orbitronics applications.

Electronic structures and Mott state of epitaxial TaS2 monolayers

Electronic structures and Mott state of epitaxial TaS2 monolayers

Two-Dimensional Moiré Polaronic Electron Crystals.

Two-dimensional moiré materials have emerged as the most versatile platform for realizing quantum phases of electrons. Here, we explore the stability origins of correlated states in WSe_{2}/WS_{2} moiré superlattices. We find that ultrafast electronic excitation leads to partial melting of the Mott states on timescales 5 times longer than predictions from the charge hopping integrals and that the melting rates are thermally activated, with activation energies of 18±3 and 13±2 meV for the one- and two-hole Mott states, respectively, suggesting significant electron-phonon coupling. A density functional theory calculation of the one-hole Mott state confirms polaron formation and yields a hole-polaron binding energy of 16meV. These findings reveal a close interplay of electron-electron and electron-phonon interactions in stabilizing the polaronic Mott insulators at transition metal dichalcogenide moiré interfaces.

Superconductivity in a Layered Cobalt Oxychalcogenide Na2CoSe2O with a Triangular Lattice.

Unconventional superconductivity in bulk materials under ambient pressure is extremely rare among the 3d transition metal compounds outside the layered cuprates and iron-based family. It is predominantly linked to highly anisotropic electronic properties and quasi-two-dimensional (2D) Fermi surfaces. To date, the only known example of a Co-based exotic superconductor is the hydrated layered cobaltate, NaxCoO2·yH2O, and its superconductivity is realized in the vicinity of a spin-1/2 Mott state. However, the nature of the superconductivity in these materials is still a subject of intense debate, and therefore, finding a new class of superconductors will help unravel the mysteries of their unconventional superconductivity. Here, we report the discovery of superconductivity at ∼6.3 K in our newly synthesized layered compound Na2CoSe2O, in which the edge-shared CoSe6 octahedra form [CoSe2] layers with a perfect triangular lattice of Co ions. It is the first 3d transition metal oxychalcogenide superconductor with distinct structural and chemical characteristics. Despite its relatively low TC, this material exhibits very high superconducting upper critical fields, μ0HC2(0), which far exceeds the Pauli paramagnetic limit by a factor of 3-4. First-principles calculations show that Na2CoSe2O is a rare example of a negative charge transfer superconductor. This cobalt oxychalcogenide with a geometrical frustration among Co spins shows great potential as a highly appealing candidate for the realization of unconventional and/or high-TC superconductivity beyond the well-established Cu- and Fe-based superconductor families and opens a new field in the physics and chemistry of low-dimensional superconductors.

Kinetic magnetism in triangular moiré materials

Magnetic properties of materials ranging from conventional ferromagnetic metals to strongly correlated materials such as cuprates originate from Coulomb exchange interactions. The existence of alternate mechanisms for magnetism that could naturally facilitate electrical control has been discussed theoretically1–7, but an experimental demonstration8 in an extended system has been missing. Here we investigate MoSe2/WS2 van der Waals heterostructures in the vicinity of Mott insulator states of electrons forming a frustrated triangular lattice and observe direct evidence of magnetic correlations originating from a kinetic mechanism. By directly measuring electronic magnetization through the strength of the polarization-selective attractive polaron resonance9,10, we find that when the Mott state is electron-doped, the system exhibits ferromagnetic correlations in agreement with the Nagaoka mechanism.

Orbital-selective metal skin induced by alkali-metal-dosing Mott-insulating Ca2RuO4

Doped Mott insulators are the starting point for interesting physics such as high temperature superconductivity and quantum spin liquids. For multi-band Mott insulators, orbital selective ground states have been envisioned. However, orbital selective metals and Mott insulators have been difficult to realize experimentally. Here we demonstrate by photoemission spectroscopy how Ca2RuO4, upon alkali-metal surface doping, develops a single-band metal skin. Our dynamical mean field theory calculations reveal that homogeneous electron doping of Ca2RuO4 results in a multi-band metal. All together, our results provide evidence for an orbital-selective Mott insulator breakdown, which is unachievable via simple electron doping. Supported by a cluster model and cluster perturbation theory calculations, we demonstrate a type of skin metal-insulator transition induced by surface dopants that orbital-selectively hybridize with the bulk Mott state and in turn produce coherent in-gap states.

Controlling dual Mott states by hydrogen doping to perovskite rare-earth nickelates

Controlling dual Mott states by hydrogen doping to perovskite rare-earth nickelates

Magnetic Field-Stabilized Wigner Crystal States in a Graphene Moiré Superlattice.

ABC-stacked trilayer graphene on boron nitride (ABC-TLG/hBN) moiré superlattices provides a tunable platform for exploring Wigner crystal states in which the electron correlation can be controlled by electric and magnetic fields. Here we report the observation of magnetic field-stabilized Wigner crystal states in a ABC-TLG/hBN. We show that correlated insulating states emerge at multiple fractional and integer fillings corresponding to ν = 1/3, 2/3, 1, 4/3, 5/3, and 2 electrons per moiré lattice site under a magnetic field. These correlated insulating states can be attributed to generalized Mott states for the integer fillings and generalized Wigner crystal states for the fractional fillings. The generalized Wigner crystal states are stabilized by a vertical magnetic field and are strongest at one magnetic flux quantum per three moiré superlattices. The ν = 2 insulating state persists up to 30 T, which can be described by a Mott-Hofstadter transition at a high magnetic field.

Emergence of damped-localized excitations of the Mott state due to disorder

A key aspect of ultracold bosonic quantum gases in deep optical lattice potential wells is the realization of the strongly interacting Mott insulating phase. Many characteristics of this phase are well understood, however little is known about the effects of a random external potential on its gapped quasiparticle and quasihole low-energy excitations. In the present study we investigate the effect of disorder upon the excitations of the Mott insulating state at zero temperature described by the Bose–Hubbard model. Using a field-theoretical approach we obtain a resummed expression for the disorder ensemble average of the spectral function. Its analysis shows that disorder leads to an increase of the effective mass of both quasiparticle and quasihole excitations. Furthermore, it yields the emergence of damped states, which exponentially decay during propagation in space and dominate the whole band when disorder becomes comparable to interactions. We argue that such damped-localized states correspond to single-particle excitations of the Bose-glass phase.

Information theoretic measures for interacting bosons in optical lattice.

This work reports the different information theoretic measures, i.e., Shannon information entropy, order, disorder, complexity, and their dynamical measure for the interacting bosons in an optical lattice with both commensurate and incommensurate filling factor. We solve the many-body Schrödinger equationfrom first principles by multiconfigurational time-dependent Hartree method which calculates all the measures with high level of accuracy. We find for both relaxed state as well as quenched state the López-Ruiz-Mancini-Calbet (LMC) measure of complexity is the most efficient depictor of superfluid (SF) to Mott-insulator transition. In the quench dynamics, the distinct structure of LMC complexity can be used as a "figureof merit" to obtain the timescale of SF to Mott state entry, Mott holding time, and the Mott state to SF state entry in the successive cycles. We also find that fluctuations in the dynamics of LMC complexity measure for incommensurate filling clearly establish that superfluid to Mott-insulator transition is incomplete. We overall conclude that distinct structure in the complexity makes it more sensitive than the standard use of Shannon information entropy.

Mottness in two-dimensional van der Waals Nb3X8 monolayers (X=Cl,Br,andI)

We investigate strong electron-electron correlation effects on two-dimensional van der Waals materials ${\mathrm{Nb}}_{3}{X}_{8} (X=\mathrm{Cl},\mathrm{Br},\phantom{\rule{0.28em}{0ex}}\text{and}\phantom{\rule{0.28em}{0ex}}\mathrm{I})$. We find that the monolayers ${\mathrm{Nb}}_{3}{X}_{8}$ are ideal systems close to the strong correlation limit. They can be described by a half-filled single band Hubbard model in which the ratio between the Hubbard, $U$, and the bandwidth, $W, U/W\ensuremath{\approx}5--10$. Both Mott and magnetic transitions of the material are calculated by the slave boson mean-field theory. Doping the Mott state, a ${d}_{{x}^{2}\ensuremath{-}{y}^{2}}+i{d}_{xy}$ superconducting pairing instability is found. We also construct a tunable bilayer Hubbard system for two sliding ${\mathrm{Nb}}_{3}{X}_{8}$ layers. The bilayer system displays a crossover between the band insulator and Mott insulator.

Confinement induced frustration in a one-dimensional lattice gauge theory

Coupling dynamical charges to gauge fields can result in highly non-local interactions with a linear confining potential. As a consequence, individual particles bind into mesons which, in one dimension, become the new constituents of emergent Luttinger liquids (LLs). Furthermore, at commensurate fillings, different Mott-insulating states can be stabilized by including nearest-neighbour (NN) interactions among charges. However, rich phase diagrams expected in such models have not been fully explored and still lack comprehensive theoretical explanation. Here, by combining numerical and analytical tools, we study a simple one-dimensional lattice gauge theory at half-filling, where U(1) matter is coupled to gauge fields and interacts through NN repulsion. We uncover a rich phase diagram where the local NN interaction stabilizes a Mott state of individual charges (or partons) on the one hand, and an LL of confined mesons on the other. Furthermore, at the interface between these two phases, we uncover a highly frustrated regime arising due to the competition between the local NN repulsion and the non-local confining interactions, realizing a pre-formed parton plasma. Our work is motivated by the recent progress in ultracold atom experiments, where such simple model could be readily implemented. For this reason we calculate the static structure factor which we propose as a simple probe to explore the phase diagram in an experimental setup.

Stable Mott Polaron State Limits the Charge Density in Lead Halide Perovskites.

Large polarons are known to form in lead halide perovskites (LHPs). Photoinduced isolated polarons at low densities have been well-researched, but many-body interactions at elevated polaron densities, exceeding the Mott criterion (i.e., Mott polaron density), have remained elusive. Here, employing ultrafast terahertz spectroscopy, we identify a stable Mott polaron state in LHPs at which the polaron wavefunctions start to overlap. The Mott polaron density is determined to be ∼1018 cm-3, in good agreement with theoretical calculations based on the Feynman polaron model. The electronic phase transition across the Mott density is found to be universal in LHPs and independent of the constituent ions. Exceeding the Mott polaron density, excess photoinjected charge carriers annihilate quickly within tens to hundreds of picoseconds, before reaching the stable and long-lived Mott state. These results have considerable implications for LHP-based devices and for understanding exotic phenomena reported in LHPs.

Superfluid density and two-component conductivity in hole-doped cuprates

While the pseudogap dominates the phase diagram of hole-doped cuprates, connecting the antiferromagnetic parent insulator at low doping to the strange metal at higher doping, its origin and relation to superconductivity remains unknown. In order to proceed, a complete understanding of how the single hole–initially localized in the Mott state–becomes mobile and ultimately evolves into a coherent quasiparticle at the end of the superconducting dome is required. In order to affect this development, we examine recent transport and spectroscopic studies of hole-doped cuprates across their phase diagram. In the process, we highlight a set of empirical correlations between the superfluid density and certain normal state properties of hole-doped cuprates that offer fresh insights into the emergence of metallicity within the CuO2 plane and its influence on the robustness of the superconducting state. We conclude by arguing that the overall behavior is best understood in terms of two distinct current-carrying fluids, only one of which dominates the superconducting condensate and is gapped out below the pseudogap endpoint at a critical hole concentration p∗.

Antiferromagnetism and chiral-[formula omitted] wave superconductivity in a honeycomb lattice close to Mott state

The antiferromagnetism (AFM) and chiral-d wave superconductivity (SC) in a honeycomb lattice close to an antiferromagnetic (AF) Mott state at half band filling are studied with a t−J model and slave boson mean field theory. The order parameters and single particle dispersion relations at different band filling fractions are investigated. It is found that the AFM enhances the SC, and leads to nodal single particle dispersion relations at two band filling fractions. These unexpected nodal dispersion relations out of nodeless chiral-d wave superconducting order are discussed. A comparison between AF chiral-d wave states and AF extended-s wave states is also given to highlight the pertinent features in chiral-d wave superconducting states. This study may be related to the honeycomb lattice materials such as the In3Cu2VO9 compound.

Quasi-Two-Dimensional Anomalous Hall Mott Insulator of Topologically Engineered Jeff=1/2 Electrons

We investigate an experimental toy-model system of a pseudospin-half square-lattice Hubbard Hamiltonian in [(SrIrO3)1/(CaTiO3)1] to include both nontrivial complex hopping and moderate electronic correlation. While the former induces electronic Berry phases as anticipated from the weak-coupling limit, the later stabilizes an antiferromagnetic (AFM) Mott insulator ground state in analogous to the strong-coupling limit. Their combined results in the real system are found to be an anomalous Hall effect with a non-monotonic temperature dependence due to the self-competition of the electron-hole pairing in the Mott state, and an exceptionally large Ising anisotropy that is captured as a giant magnon gap beyond the superexchange approach. The unusual phenomena highlight the rich interplay of electronic topology and electronic correlation in the intermediate-coupling regime that is largely unexplored and challenging in theoretical modelling.

Trigonal symmetry breaking and its electronic effects in the two-dimensional dihalides MX2 and trihalides MX3

We study the consequences of the approximately trigonal (${D}_{3d}$) point symmetry of the transition metal ($M$) site in two-dimensional van der Waals ${MX}_{2}$ dihalides and ${MX}_{3}$ trihalides. The trigonal symmetry leads to a 2-2-1 orbital splitting of the transition metal $d$ shell, which is best represented by $d$ orbitals that describe the trigonal rather than ${O}_{h}$ symmetry. The ligand-ligand bond length differences (rather than metal-ligand) take the role of a Jahn-Teller-like mode and in combination with interlayer distances and dimensionality effects tune the crystal field splittings and bandwidths. These effects, in turn, are amplified by electronic correlation effects---leading to crystal field splittings of the order of 0.1--1 eV between the singlet and the lowest orbital doublet---as opposed to the often assumed degenerate $3\phantom{\rule{0.16em}{0ex}}{t}_{2g}$ states. Our calculations explain why most of the materials in this family are insulating, and why these considerations have to be taken into account in realistic models of them. Further, orbital order coupled to various lower symmetry lattice modes may lift the remaining orbital degeneracies, and we explain how these may support unique electronic states using ${\mathrm{ZrI}}_{2}$ and ${\mathrm{CuCl}}_{2}$ as examples, and offer a brief overview of possible electronic configurations in this class of materials. By building and analyzing Wannier models adapted to the appropriate symmetry we examine how the interplay among trigonal symmetry, electronic correlation effects, and $p\text{\ensuremath{-}}d$ orbital charge transfer leads to insulating, orbitally polarized magnetic and/or orbital-selective Mott states, and we provide a simple framework and numerical tool for others. Our paper establishes a rigorous framework to understand, control, and tune the electronic states in low-dimensional correlated halides. Our analysis shows that trigonal symmetry and its breaking is a key feature of the two-dimensional halides that needs to be accounted for in search of novel electronic states in materials ranging from ${\mathrm{CrI}}_{3}$ to $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$.