Mott Physics Research Articles

Mott Transitions: A Brief Review

AbstractThis short review provides an overview of some aspects of the current understanding of Mott insulators and Mott metal‐insulator transitions. The development of this field is traced, from earliest classical views to the state‐of‐the‐art picture based on methods of quantum field theory. A quasi‐local view point, characterizing “pure” Mott physics, throughout this article is focused on. Following an extensive discussion on Mott transitions in one‐ and multi‐orbital Hubbard models, progress is reviewed in first‐principles correlation‐based approaches in achieving a quantitative description of insulator‐metal transitions in two celebrated Mott materials. Building thereupon, success of such approaches in providing microscopic justification for the famed Mott criterion, as well as in the attempts to model emerging devices is reviewed briefly. The study is concluded with a discussion of a class of Mott insulators modeled by the Kugel‐Khomskii model, and discuss how progress in the understanding of novel quantum liquid‐crystal‐like order provides an attractive opportunity to gain insight into topologically ordered states and topological‐to‐trivial phase transitions for certain quantum spin models in terms of a dual description in terms of Landau‐like symmetry breaking.

Superconductivity and Mott Physics in Organic Charge Transfer Materials.

The phase diagrams of quasi two-dimensional organic superconductors display a plethora of fundamental phenomena associated with strong electron correlations, such as unconventional superconductivity, metal-insulator transitions, frustrated magnetism and spin liquid behavior. We analyze a minimal model for these compounds, the Hubbard model on an anisotropic triangular lattice, using cutting-edge quantum embedding methods respecting the lattice symmetry. We demonstrate the existence of unconventional superconductivity by directly entering the symmetry-broken phase. We show that the crossover from the Fermi liquid metal to the Mott insulator is associated with the formation of a pseudogap. The predicted momentum-selective destruction of the Fermi surface into hot and cold regions provides motivation for further spectroscopic studies. Our theoretical results agree with experimental phase diagrams of κ-BEDT organics.

Mott-Insulator State of FeSe as a Van der Waals 2D Material Is Unveiled.

We undertook a comprehensive investigation of the electronic structure of FeSe, known as a Hund metal, and found that it is not uniquely defined. Through accounting for all two-particle irreducible diagrams constructed from electron Green's function G and screened Coulomb interaction W in a self-consistent manner, a Mott-insulator phase of 2D-FeSe is unveiled. The metal-insulator transition is driven by the strong on-site Coulomb interaction in its paramagnetic phase, accompanied by the weakening of both local and nonlocal screening effects on the Fe-3d orbitals. Our results suggest that Mott physics may play a pivotal role in shaping the electronic, optical, and superconducting properties of monolayer or nanostructured FeSe.

Dual nature of magnetism driven by momentum dependent f-d Kondo hybridization

The intricate nature of magnetism in uranium-based Kondo lattices is a consequence of correlations between U-5f and conduction electrons. Previously, the source of magnetism has been ascribed to either Mott physics or Ruderman-Kittel-Kasuya-Yosida interaction, both of which are not fully applicable to uranium-based Kondo lattices. Using linearized quasiparticle self-consistent GW plus dynamical mean-field theory, we demonstrate a crossover from incoherent to coherent f-d Kondo cloud in the paramagnetic phase of UTe2, USbTe and USbSe. As the transition occurs, we observe an augmented f-d coherence and Pauli-like magnetic susceptibility, with a substantial frozen magnetic moment of U-5f persisting. We show that momentum dependent f-d hybridization is responsible for the magnetic moments arising from the renormalized f electrons’ van Hove singularity. Our findings provide a perspective to explain the dual nature of magnetism and the long-range magnetic ordering induced by pressure in UTe2.

Phonon Thermal Transport in UO_{2} via Self-Consistent Perturbation Theory.

Computing thermal transport from first-principles in UO_{2} is complicated due to the challenges associated with Mott physics. Here, we use irreducible derivative approaches to compute the cubic and quartic phonon interactions in UO_{2} from first principles, and we perform enhanced thermal transport computations by evaluating the phonon Green's function via self-consistent diagrammatic perturbation theory. Our predicted phonon lifetimes at T=600 K agree well with our inelastic neutron scattering measurements across the entire Brillouin zone, and our thermal conductivity predictions agree well with previous measurements. Both the changes due to thermal expansion and self-consistent contributions are nontrivial at high temperatures, though the effects tend to cancel, and interband transitions yield a substantial contribution.

Composition-driven Mott transition within SrTi 1−x V x O3

The last few decades has seen the rapid growth of interest in the bulk perovskite-type transition metal oxides SrVO3 and SrTiO3. The electronic configuration of these perovskites differs by one electron associated to the transition metal species which gives rise to the drastically different electronic properties. Therefore, it is natural to look into how the electronic structure transitions between these bulk structures by using doping. Measurements of the substitutional doped SrTi 1−x V x O3 shows an metal–insulator transition (MIT) as a function of doping. By using supercell density functional theory with dynamical mean field theory (DFT+DMFT), we show that the MIT is indeed the result of the combination of local electron correlation effects (Mott physics) within the t2g orbitals and the atomic site configuration of the transition metals which may indicate dependence on site disorder. SrTi 1−x V x O3 may be an ideal candidate for benchmarking cutting-edge Mott–Anderson models of real systems. We show that applying an effective external perturbation on SrTi 1−x V x O3 can switch the system between the insulating and metallic phase, meaning this is a bulk system with the potential use in Mott electronic devices.

Charge-Density-Wave Order And Electronic Phase Transitions in a Dilute D-Band Semiconductor.

As one of the most fundamental physical phenomena, charge density wave (CDW) order predominantly occurs in metallic systems such as quasi-one-dimensional (quasi-1D) metals, doped cuprates, and transition metal dichalcogenides, where it is well understood in terms of Fermi surface nesting and electron-phonon coupling mechanisms. On the other hand, CDW phenomena in semiconducting systems, particularly at the low carrier concentration limit, are less common and feature intricate characteristics, which often necessitate the exploration of novel mechanisms, such as electron-hole coupling or Mott physics, to explain. In this study, we combined electrical transport, synchrotron X-ray diffraction and density-functional theory (DFT) calculations to investigate CDW order and a series of hysteretic phase transitions in a dilute d-band semiconductor, BaTiS3 . Our experimental and theoretical findings suggest that the observed CDW order and phase transitions in BaTiS3 may be attributed to both electron-phonon coupling and non-negligible electron-electron interactions in the system. Our work highlights BaTiS3 as a unique platform to explore CDW physics and novel electronic phases in the dilute filling limit and could open new opportunities for developing novel electronic devices. This article is protected by copyright. All rights reserved.

Orbital-selective altermagnetism and correlation-enhanced spin-splitting in strongly-correlated transition metal oxides

We investigate the altermagnetic properties of strongly-correlated transition metal oxides considering the family of the quasi two-dimensional A2BO4 and three-dimensional ABO3. As a test study, we analyze the Mott insulators Ca2RuO4 and YVO3. In both cases, the orbital physics is extremely relevant in the t2g subsector with the presence of an orbital-selective Mott physics in the first case and of a robust orbital-order in the second case. Using first-principles calculations, we show the presence of an orbital-selective altermagnetism in the case of Ca2RuO4. In the case of YVO3, we study the altermagnetism as a function of the magnetic ordering and of the Coulomb repulsion U. We find that the altermagnetism is present in all magnetic orders with the symmetries of the Brillouin zone depending on the magnetic order. Finally, the Coulomb repulsion enhances the non-relativistic spin-splitting making the strongly-correlated systems an exciting playground for the study of the altermagnetism.

Observation of Electronic Strong Correlation in VTe_{2}-2sqrt[3]×2sqrt[3] Monolayer.

Strong electron correlation under two-dimensional limit is intensely studied in the transition metal dichalcogenides monolayers, mostly within their charge density wave (CDW) states that host a star of David period. Here, by using scanning tunneling microscopy and spectroscopy and density functional theory calculations with on-site Hubbard corrections, we study the VTe_{2} monolayer with a different 2sqrt[3]×2sqrt[3] CDW period. We find that the dimerization of neighboring Te-Te and V-V atoms occurs during the CDW transition, and that the strong correlation effect opens a Mott-like full gap at Fermi energy (E_{F}). We further demonstrate that such a Mott phenomenon is ascribed to the combination of the CDW transition and on-site Coulomb interactions. Our work provides a new platform for exploring Mott physics in 2D materials.

Bandwidth Control and Symmetry Breaking in a Mott‐Hubbard Correlated Metal

AbstractIn Mott materials strong electron correlation yields a spectrum of complex electronic structures. Recent synthesis advancements open realistic opportunities for harnessing Mott physics to design transformative devices. However, a major bottleneck in realizing such devices remains the lack of control over the electron correlation strength. This stems from the complexity of the electronic structure, which often veils the basic mechanisms underlying the correlation strength. This study presents control of the correlation strength by tuning the degree of orbital overlap using picometer‐scale lattice engineering. This study illustrates how bandwidth control and concurrent symmetry breaking can govern the electronic structure of a correlated SrVO3 model system. This study shows how tensile and compressive biaxial strain oppositely affect the SrVO3 in‐plane and out‐of‐plane orbital occupancy, resulting in the partial alleviation of the orbital degeneracy. The spectral weight redistribution under strain is derived and explained, which illustrates how high tensile strain drives the system toward a Mott insulating state. Implementation of such concepts can push correlated electron phenomena closer toward new solid‐state devices and circuits. These findings therefore pave the way for understanding and controlling electron correlation in a broad range of functional materials, driving this powerful resource for novel electronics closer toward practical realization.

Positive and Negative Pressure Regimes in Anisotropically Strained V2O3 Films

AbstractThe metal‐insulator phase transitions in V2O3 are considered archetypal manifestations of Mott physics. Despite decades of research, the effects of doping, pressure, and anisotropic strains on the transitions are still debated. To understand how these parameters control the transitions, anisotropically strained pure V2O3 films are explored with nearly the same contraction along the c‐axis, but different degrees of ab‐plane expansion. With small ab‐plane expansion, the films behave similar to bulk V2O3 under hydrostatic pressure. However, with large ab‐plane expansion, the films are driven into the “negative pressure” regime, similar to that of Cr‐doped V2O3, exhibiting clear coexistence of paramagnetic insulator and paramagnetic metal phases between 180–500 K. This shows that c‐axis contraction alone, or an increase in c/a ratio is insufficient for inducing “negative pressure” effects. Actually, c‐axis contraction alone destabilizes the two insulating phases of V2O3, whereas a‐axis expansion tends to stabilize them. The effects of strain are modeled using density functional theory providing good agreement with experimental results. The findings show that chemical pressure alone cannot account for the phase diagram of (V1−xCrx)2O3. This work enables to manipulate a Mott transition above room temperature, thereby expanding the opportunities for applications of V2O3 in novel electronics.

Fractional topology in interacting one-dimensional superconductors

We investigate the topological phases of two one-dimensional (1D) interacting superconducting wires and propose topological markers directly measurable from ground-state correlation functions. These quantities remain powerful tools in the presence of couplings and interactions. We show with the density matrix renormalization group that the double critical Ising (DCI) phase of two interacting Kitaev chains is a fractional topological phase with gapless Majorana modes in the bulk, and a one-half topological invariant per wire. Using both numerics and quantum field theoretical methods, we show that the phase diagram remains stable in the presence of an interwire hopping amplitude ${t}_{\ensuremath{\perp}}$ at length scales below $\ensuremath{\sim}1/{t}_{\ensuremath{\perp}}$. A large interwire hopping amplitude results in the emergence of two integer topological phases, stable also at large interactions. They host one edge mode per boundary shared between both wires. At large interactions, the two wires are described by Mott physics, with the ${t}_{\ensuremath{\perp}}$ hopping amplitude resulting in a paramagnetic order.

Observation of Mott instability at the valence transition of f-electron system.

Mott physics plays a critical role in materials with strong electronic correlations. Mott insulator-to-metal transition can be driven by chemical doping, external pressure, temperature and gate voltage, which is often seen in transition metal oxides with 3d electrons near the Fermi energy (e.g. cuprate superconductor). In 4f-electron systems, however, the insulator-to-metal transition is mostly driven by Kondo hybridization and the Mott physics has rarely been explored in experiments. Here, by combining the angle-resolved photoemission spectroscopy and strongly correlated band structure calculations, we show that an unusual Mott instability exists in YbInCu4 accompanying its mysterious first-order valence transition. This contrasts with the prevalent Kondo picture and demonstrates that YbInCu4 is a unique platform to explore the Mott physics in Kondo lattice systems. Our work provides important insight for the understanding and manipulation of correlated quantum phenomena in the f-electron system.

Threshold-like Superlinear Accumulation of Excitons in a Gated Monolayer Transition Metal Dichalcogenide

Coexistence and mutual conversion of various excitonic species in semiconductors are the essence of Mott physics and underpin important device applications such as excitonic or polaritonic lasers. The emergence of monolayer semiconductors provides unprecedented opportunities to study these fundamental issues due to the much larger exciton binding energies. In this paper, we study the evolution of the coupled exciton–trion system in electrically gated monolayer MoTe2 devices. Contrary to the conventional linear scaling, we found that exciton density exhibits an abnormal three-stage scaling behavior: a conventional linear scaling at low pumping levels, followed by a superlinear behavior accompanied by a strong saturation of trion emission. In the third stage, the exciton emission returns to the linear scaling with the further increase of pumping. Although such behavior has a rare similarity in other physical systems, surprisingly we discovered a complete analogy of this behavior with the threshold of a conventional laser and proved mathematically that the exciton–trion equations are identical to the laser equations. We further showed that the power-law index increases with the charge density experimentally and can be as high as 40 at a density of ∼1 × 1012/cm2 in principle, leading to extremely nonlinear behavior of exciton accumulation. Our results reveal a new behavior of exciton accumulation and provide an alternative mechanism for multiplying exciton population, in analogy to a condensate. The intricate dynamics between excitons and trions will also enrich our understanding of the complex Mott physics in 2D semiconductors and may lead to new devices based on the exciton nonlinearity.

Mott physics: One of main themes in quantum materials

<sec>The competition and cooperation between the itinerancy behavior and localization behavior of electrons in correlated quantum materials, known as Mott physics, is the physical mechanism behind the diverse states of many quantum materials. This article reviews the manifestation of Mott physics in various quantum materials and establishes it as one of the main themes of quantum materials. Finding and understanding its ever-changing ways of manifestation is one of the central tasks of experimental research on condensed matter physics.</sec><sec>Specifically, the filling-control route of Mott transition is illustrated by exampling the surface K-dosed Sr<sub>2</sub>IrO<sub>4</sub>, which exhibits d-wave gap, pseudogap behavior in underdoped regime, and phase separation with inhomogeneous electronic state distribution. All of these show strong resemblances to the doped cuprate superconductors, another prototypical filling-control type of Mott transition case. On the other hand, the bandwidth-control route of Mott transition could be found in NiS<sub>2–<i>x</i></sub>Se<sub><i>x</i></sub>, where its bandwidth continuously decreases with decreasing Se concentration, until it becomes an insulator. In addition, the essence of various ways of doping in iron-based superconductors is to change their bandwidths. The superconductivity shows up at intermediate bandwidth with moderate correlations, and it diminishes when the bandwidth is large and the electron correlations are weak. For heavily electron-doped iron-selenides, there is even a Mott insulator phase with strong correlations.</sec><sec>For carbon based materials, the phase transition between the antiferromagnetic insulator and superconducting state of A15 Cs<sub>3</sub>C<sub>60</sub> as the volume of fullerene anions decreases could be understood in terms of a bandwidth-control Mott transition; the insulator-superconductor transition discovered in electrically gated “magic angle” twisted-angle bilayer graphene could be understood as a filling-control Mott transition.</sec><sec>For f electron systems, the interplay between itinerancy and localization dominates the heavy fermion behavior and their ground states. The behaviors of the f electrons are demonstrated by using the angle-resolved photoemission data of CeCoIn<sub>5</sub>, whose f electron band becomes more coherent with decreasing temperature, and the c-f hybridization is thus enhanced and the band mass of conduction band continuously increases. The c-f hybridization behaviors of CeCoIn<sub>5,</sub> CeIrIn<sub>5</sub>, and CeRhIn<sub>5</sub> are compared with each other, and the differences in hybridization strength put their ground states into different regimes of the Doniach phase diagram. Similarly, the Skutterudites 4f<sup>2</sup> Kondo lattice system PrOs<sub>4</sub>Sb<sub>12</sub> and its sibling 4f<sup>1</sup> system CeOs<sub>4</sub>Sb<sub>12</sub> also have different ground states due to a slight difference in their c-f hybridization strengths.</sec>

Metal–insulator transitions in dimensionality controlled LaxSr1−xVO3 films

Carrier doping into two dimensional (2D) Mott insulators is one of the prospective strategies for exploring exotic quantum phenomena. Although ultra-thin oxide films are one such target, it is vitally important to fabricate well-defined and clean samples to extract intrinsic properties. In this study, we start from establishing the growth of clean SrVO3 films with a low residual resistivity (∼4 × 10−7 Ω cm) and a high mobility (∼103 cm2/V s). By confining them with SrTiO3 barrier layers, the Mott insulator state appears at the thickness below 3 unit cells (u.c.). By the electron doping in the form of LaxSr1−xVO3 for such two dimensional systems (2 and 3 u.c), metallic-like phases appear in a narrow x region around x = 0.17, indicating a collapse of the Mott insulator state. This study demonstrates that artificial 2D systems of clean oxides are a promising playground for exploring novel Mott physics in confined systems.

Charge Transport in Ba1−xRbxFe2As2 Single Crystals

Recent studies in heavily hole-doped iron-based superconductor RbFe$_2$As$_2$ have suggested the emergence of novel electronic nematicity directed along the Fe-As direction, 45$^\circ$ rotated from the usual nematicity ubiquitously found in BaFe$_2$As$_2$ and related materials. This motivates us to study the physical properties of Ba$_{1-x}$Rb$_{x}$Fe$_{2}$As$_{2}$, details of which remain largely unexplored. Here we report on the normal-state charge transport in Ba$_{1-x}$Rb$_{x}$Fe$_{2}$As$_{2}$ superconductors by using high-quality single crystals in the range of Rb concentration $0.14\le x \le 1.00$. From the systematic measurements of the temperature dependence of electrical resistivity $\rho(T)$, we find a signature of a deviation from the Fermi liquid behavior around the optimal composition, which does not seem related to the antiferromagnetic quantum criticality but has a potential link to hidden nematic quantum criticality. In addition, electron correlations derived from the coefficient of $T^2$ resistivity show a marked increase with Rb content near the heavily hole-doped end, consistent with the putative Mott physics near the $3d^5$ electron configuration in iron-based superconductors.

Flavour-selective localization in interacting lattice fermions

A large repulsion between particles in a quantum system can lead to their localization, an effect responsible for the Mott insulator phases in strongly correlated materials. In a system with multiple orbitals, an orbital-selective Mott insulator can form, where electrons in some orbitals are predicted to localize while others remain itinerant. Here we demonstrate a more general version of this phenomenon by observing flavour-selective localization in an atom-based quantum simulator. Our experiment realizes Fermi–Hubbard models with an SU(3) symmetry that can be broken using a tunable coupling between flavours. We observe an enhancement of the localization associated with a selective Mott transition and the emergence of flavour-dependent correlations. Our realization of flavour-selective Mott physics demonstrates the potential of cold atoms to simulate interacting multicomponent materials such as superconductors and topological insulators.

Capturing the ground state of uranium dioxide from first principles: Crystal distortion, magnetic structure, and phonons

Uranium dioxide (UO$_2$) remains a formidable challenge for first-principles approaches, due to the complex interplay among spin-orbit coupling, Mott physics, magnetic ordering, and crystal distortions. Here we use DFT+$U$ to explore UO$_2$ at zero temperature, incorporating all the aforementioned phenomena. The technical challenge is to navigate the many metastable electronic states produced by DFT+$U$, which is acomplished using $f$-orbital occupation matrix control to search for the ground state. We restrict our search to the high-symmetry ferromagnetic phase, including spin-orbit coupling, which produces a previously unreported occupation matrix. This newfound occupation matrix is then used as an initialization to explore the broken symmetry phases. We find the oxygen cage distortion of the 3k antiferromagnetic state to be in excellent agreement with experiments, and both the spin-orbit coupling and the Hubbard $U$ are critical ingredients. We demonstrate that only select phonon modes have a strong dependence on the Hubbard $U$, whereas magnetic ordering has only a small influence overall. We perform measurements of the phonon dispersion curves using inelastic neutron scattering, and our calculations show good agreement when using reasonable values of $U$. The quantitative success of DFT+$U$ warrants exploration of thermal transport and other observables within this level of theory.

Mott correlations in ABC graphene trilayer aligned with hBN

ABC trilayer graphene aligned with hexagonal boron nitride (ABC/hBN) and other moir\'e systems have shown insulating phases at integer fillings of the moir\'e lattice. The role of Mott physics in these insulating states has been questioned by observations of correlated states in a nonaligned ABC trilayer, but recent photocurrent experiments in aligned samples are consistent with the existence of a Mott insulating state at half filling. Using dynamical mean-field theory we address the effect of Mott correlations in ABC/hBN. We show that, at experimentally relevant interaction values, the electronic states are strongly affected by a significant spectral weight transfer not present without alignment to hBN. This effect, which emerges at interactions considerably smaller than ${U}_{\mathrm{Mott}}$ (at which the Mott metal-insulator transition takes place) and does not require symmetry breaking, also impacts the electronic properties at temperatures above the ordering transitions producing anomalous temperature and doping dependencies. Close to the Mott transition, the intramoir\'e unit cell interactions promote an antiferromagnetic state, probably breaking the ${C}_{3}$ symmetry, that would compete with the ferromagnetic exchange interactions to determine the ground state.