We develop a theory of the excitonic phase recently proposed as the zero-field insulating state observed near charge neutrality in monolayer WTe$_2$. Using a Hartree-Fock approximation, we numerically identify two distinct gapped excitonic phases: a spin density wave state for weak non-zero interaction strength and spin spiral order at stronger interactions, separated by a narrow window of non-excitonic quantum spin Hall insulator. We introduce a simplified model capturing key features of the WTe$_2$ band structure, in which these phases appear as distinct valley ferromagnetic orders. We link the competition between the excitonic phases to the orbital structure of electronic wavefunctions at the Fermi surface and hence its proximity to the underlying gapped Dirac point in WTe$_2$. We briefly discuss collective modes of the two excitonic states, and comment on implications for experiments.
Recently, quantum oscillation of the resistance in insulating monolayer WTe$_2$ was reported. An explanation in terms of gap modulation in the hybridized Landau levels of an excitonic insulator was also proposed by one of us. However, the previous picture of gap modulation in the Landau levels spectrum was built on a pair of well nested electron and hole Fermi surfaces, while the monolayer WTe$_2$ has one hole and two electron Fermi pockets with relative anisotropy. Here we demonstrate that for system like monolayer WTe$_2$, the excitonic insulating state arising from the coupled one hole and …
A recent paper on the insulating state of monolayer WTe2 reported the observation of large oscillations in the conductivity that are periodic in 1/B, resembling quantum oscillations in metals. This remarkable observation has inspired suggestions of exotic physics such as spin-charge separation. We show that a rather more conventional but still nontrivial explanation in terms of gap modulation may be possible in a model of excitonic insulator subject to a magnetic field.
A sufficiently strong Coulomb interaction may open an excitonic fermion gap and thus drive a semimetal-insulator transition in graphene. In this paper, we study the Eliashberg theory of excitonic transition by coupling the fermion gap equation self-consistently to the equation of vacuum polarization function. Including the fermion gap into polarization function increases the effective strength of Coulomb interaction because it reduces the screening effects due to the collective particle-hole excitations. Although this procedure does not change the critical point, it leads to a significant enha…
The competing ground states of bilayer graphene are studied by applying renormalization group techniques to a bilayer honeycomb lattice with nearest neighbor hopping. In the absence of interactions, the Fermi surface of this model at half-filling consists of two nodal points with momenta $\mathbf{K}$, $\mathbf{K}'$, where the conduction band and valence band touch each other, yielding a semi-metal. Since near these two points the energy dispersion is quadratic with perfect particle-hole symmetry, excitonic instabilities are inevitable if inter-band interactions are present. Using a perturbativ…
The strong long-range Coulomb interaction between massless Dirac fermions in graphene can drive a semimetal-insulator transition. We show that this transition is strongly suppressed when the Coulomb interaction is screened by such effects as disorder, thermal fluctuation, doping, and finite volume. It is completely suppressed once the screening factor $μ$ is beyond a threshold $μ_{c}$ even for infinitely strong coupling. However, such transition is still possible if there is an additional strong contact four-fermion interaction. The differences between screened and contact interactions are als…
The interplay between topology and correlations can generate a variety of quantum phases, many of which remain to be explored. Recent advances have identified monolayer WTe2 as a promising material for doing so in a highly tunable fashion. The ground state of this two-dimensional (2D) crystal can be electrostatically tuned from a quantum spin Hall insulator (QSHI) to a superconductor. However, much remains unknown about the gap-opening mechanism of the insulating state. Here we report evidence that the QSHI is also an excitonic insulator (EI), arising from the spontaneous formation of electron…
Optical responses in an excitonic insulating (EI) system with strong electron correlation are studied. We adopt the two-orbital Hubbard model with a finite energy difference between the two orbitals where the spin state degree of freedom exists. This model is analyzed by the variational cluster approach. In order to include the local electron correlation effect, the vertex correction is taken into account in the formulation of the optical conductivity spectra. We calculate a finite-temperature phase diagram, in which an EI phase appears between a low-spin band insulating state and a high-spin …
A sufficiently strong long-range Coulomb interaction can induce excitonic pairing in gapless Dirac semimetals, which generates a finite gap and drives semimetal-insulator quantum phase transition. This phenomenon is in close analogy to dynamical chiral symmetry breaking in high energy physics. In most realistic Dirac semimetals, including suspended graphene, Coulomb interaction is too weak to open an excitonic gap. The Coulomb interaction plays a more important role at low energies in a two-dimensional semi-Dirac semimetal, in which the fermion spectrum is linear in one component of momenta an…
Excitonic insulating system is studied from the viewpoints of the orbital physics in strongly correlated electron systems. An effective model Hamiltonian for low-energy electronic states is derived from the two-orbital Hubbard model with a finite energy difference corresponding to the crystalline field splitting. The effective model is represented by the spin operators and the pseudo-spin operators for the spin-state degrees of freedom. The ground state phase diagram is analyzed by the mean-field approximation. In addition to the low-spin state and high-spin state phases, two kinds of the exci…
We present an $\textit{ab initio}$ study of the excitonic states of a prototypical high-temperature superconductor La$_2$CuO$_4$ and compare them to the isostructural single-layer nickelate La$_2$NiO$_4$. Key difference in the low-energy electronic structure leads to very different excitonic behavior. Excitons in La$_2$CuO$_4$ are delocalized and can freely move in the CuO$_2$ plane without disturbing the antiferromagnetic order. In contrast, in La$_2$NiO$_4$ we find the low-lying excitonic states to be extremely localized, producing a nearly flat dispersion. The theoretically obtained exciton…
Pezzini et al. reported an unconventional mass enhancement in topological nodal line semimetal ZrSiS (Nat. Phys. 14, 178 (2018), whose origin remains puzzling. In this material, strong short-range interactions might induce excitonic particle-hole pairs. Here we study the renormalization of fermion velocities and find that the mass enhancement in ZrSiS can be well understood if we suppose that ZrSiS is close to the quantum critical point between semimetal and excitonic insulator. Near this quantum critical point, the fermion velocities are considerably reduced by excitonic quantum fluctuation, …
Motivated by recent experiments, which give strong evidence for an excitonic insulating phase in $\rm TmSe_{0.45}Te_{0.55}$, we developed a scheme to quantitatively construct, for generic two-band models, the phase diagram of an excitonic insulator. As a first application of our approach, we calculated the phase diagram for an effective mass two-band model with long-range Coulomb interaction. The shielded potential approximation is used to derive a generalized gap equation controlling for positive (negative) energy gaps the transition from a semi-conducting (semi-metallic) phase to an insulati…
Effects of the spin-orbit coupling (SOC) and magnetic field on excitonic insulating (EI) states are investigated. We introduce the two-orbital Hubbard model with the crystalline field splitting, which is a minimal model for discussing the exciton condensation in strongly correlated electron systems, and analyze its effective Hamiltonian in the strong correlation limit by using the mean-field theory. In the absence of the SOC and magnetic field, the ground state changes from the nonmagnetic band-insulating state to the EI state by increasing the Hund coupling. In an applied magnetic field, the …
We propose a mechanism of the spin Seebeck effect attributed to excitonic condensation in a nonmagnetic insulator. We analyze a half-filled two-orbital Hubbard model with a crystalline field splitting in the strong coupling limit. In this model, the competition between the crystalline field and electron correlations brings about an excitonic insulating state, where the two orbitals are spontaneously hybridized. Using the generalized spin-wave theory and Boltzmann transport equation, we find that a spin current generated by a thermal gradient is observed in the excitonic insulating state withou…
We study the quantum criticality of the phase transition between the Dirac semimetal and the excitonic insulator in two dimensions. Even though the system has a semimetallic ground state, there are observable effects of excitonic pairing at finite temperatures and/or finite energies, provided that the system is in proximity to the excitonic insulating transition. To determine the quantum critical behavior, we consider three potentially important interactions, including the Yukawa coupling between Dirac fermions and the excitonic order parameter fluctuation, the long-range Coulomb interaction, …
Strong magnetic field induces at least two phase transitions in graphite beyond the quantum limit where many-body effects are expected. We report on a study using a state-of-the-art non-destructive magnet allowing to attain 90.5 T at 1.4 K, which reveals a new field-induced phase and evidence that the insulating state destroyed at 75 T is an excitonic condensate of electron-hole pairs. By monitoring the angle dependence of in-plane and out-of-plane magnetoresistance, we distinguish between the role of cyclotron and Zeeman energies in driving various phase transitions. We find that, with the no…
Tuning many-body electronic phases by an external handle is of both fundamental and practical importance in condensed matter science. The tunability mirrors the underlying interactions, and gigantic electric, optical and magnetic responses to minute external stimuli can be anticipated in the critical region of phase change. The excitonic insulator is one of the exotic phases of interacting electrons, produced by the Coulomb attraction between a small and equal number of electrons and holes, leading to the spontaneous formation of exciton pairs in narrow-gap semiconductors/semimetals. The layer…
The excitonic insulator is an elusive electronic phase exhibiting a correlated excitonic ground state. Materials with such a phase are expected to have intriguing properties such as excitonic high-temperature superconductivity. However, compelling evidence on the experimental realization is still missing. Here, we theoretically propose hybrids of two-dimensional semiconductors functionalized by organic molecules as prototypes of excitonic insulators, with the exemplary candidate WS$_2$-F6TCNNQ. This material system exhibits an excitonic insulating phase at room temperature with a ground state …
Two-dimensional (2D) moire materials provide a new solid-state platform with unprecedented controllability for studies of correlated quantum phenomena. To date, experimental studies have focused on the correlated electronic states; the correlated bosonic states in moire materials have remained practically unexplored. Here, we report a correlated dipolar excitonic insulator, a charge insulating state driven by the formation of excitons, in a Coulomb-coupled WSe2 monolayer and WSe2/WS2 moire bilayer at total hole doping density equal to the moire density. The system is a Mott insulator when all …
We study the excitonic insulating (EI) phase in the two-band Hubbard models on the Penrose tiling. Performing the real-space mean-field calculations systematically, we obtain the ground state phase diagrams for the vertex and center models. We find that, in some regimes, the stable EI phase is induced by small interband interactions. We argue that this originates from the electron-hole pairing for the completely or nearly degenerate states, which are characteristic of the Penrose tiling. We also study spatial distribution of the order parameter, mapping it to the perpendicular space.
The capability to switch electrically between superconducting and insulating states of matter represents a novel paradigm in the state-of-the-art engineering of correlated electronic systems. An exciting possibility is to turn on superconductivity in a topologically non-trivial insulator, which provides a route to search for non-Abelian topological states. However, existing demonstrations of superconductor-insulator switches have involved only topologically trivial systems, and even those are rare due to the stringent requirement to tune the carrier density over a wide range. Here we report re…
Artificial moiré superlattices in 2d van der Waals heterostructure is a new venue for realizing and controlling correlated electronic phenomena. Recently, twisted bilayer WSe$_2$ emerged as a new robust moiré system hosting a correlated insulator at moiré half-filling over a range of twist angle. In this work, we present a theory of this insulating state as an excitonic density wave due to intervalley electron-hole pairing. We show that exciton condensation is strongly enhanced by a van Hove singularity near the Fermi level. Our theory explains the remarkable sensitivity of the insulating gap …
We show that double-layer graphene (DLG), where an external potential induces an charge-imbalance between $n$- and $p$-type layers, is a promising candidate to realize an exciton condensate in equilibrium. To prove this phenomenon experimentally, we suggest to couple two DLG systems, separated by a thin insulating barrier, and measure the excitonic Josephson effect. For this purpose we calculate the ac and dc Josephson currents induced by tunneling excitons and show that the former only occurs when the gate potentials of the DLG systems differ, irrespective of the phase relationship of their e…
Excitonic insulator (EI) was proposed in 60's as a distinct insulating state originating from pure electronic interaction, but its material realization has been elusive with extremely few material candidates and with only limited evidence such as anomalies in transport properties, band dispersions, or optical transitions. We investigate the real-space electronic states of the low temperature phase in Ta$_2$NiSe$_5$ with an atomic resolution to clearly identify the quasiparticle energy gap together with the strong electron-hole band renormalization using scanning tunneling microscopy (STM) and …
The two-dimensional, colossal magnetoresistive system GdI_2 develops an unusual metallic state below its ferromagnetic transition and becomes insulating at low temperatures. It is argued that this geometrically frustrated, correlated poor metal is a possible candidate for a ferromagnetic excitonic liquid. The renormalized Fermi surface supports a further breaking of symmetry to a charge ordered, excitonic solid ground state at lower temperatures via order by disorder mechanism. Several experimental predictions are made to investigate this unique orbitally correlated ground state.
Two-dimensional Dirac fermions are subjected to two types of interactions, namely the long-range Coulomb interaction and the short-range on-site interaction. The former induces excitonic pairing if its strength $α$ is larger than some critical value $α_c$, whereas the latter drives an antiferromagnetic Mott transition when its strength $U$ exceeds a threshold $U_c$. Here, we study the impacts of the interplay of these two interactions on excitonic pairing with the Dyson-Schwinger equation approach. We find that the critical value $α_c$ is increased by weak short-range interaction. As $U$ incre…
Slave rotor mean field (SRMF) theory is employed to study exciton formation in the extended Falicov-Kimball Model (EFKM). In this theory, charge and spin (or orbital) degrees are treated as independent degrees of freedom, coupled by a constraint. Using this formalism in single as well as cluster extension, we capture the effective many body scales beyond conventional mean-field theory. While the formation of exciton is favored by the interband hybridization $V$, it is strongly influenced by the on-site Coulomb interaction $U$. Beyond a critical hybridization, there is a condensation of exciton…
Magnetic field (H) effects on a correlated electron system with the spin-state degree of freedom are examined. The effective Hamiltonian derived from the two-orbital Hubbard model is analyzed by the mean-field approximation. Applying H to the low-spin (LS) phase induces the excitonic insulating phase, as well as the spin-state ordered phase where the LS and high-spin (HS) states are ordered alternately. In the case where H is applied to the HS phase, a reentrant transition for the HS phase appears. A rich variety of the phase diagrams are attributed to the spin-state degree of freedom and thei…
We present the results of the Monte-Carlo simulation of graphene-like statistical model in terms of occupation numbers. We study the problem of the phase transition in graphene to an insulating phase. Only antiferromagnetic order parameter was studied at the moment by means of Hybrid Monte-Carlo process on the hexagonal lattice because of the sign problem for excitonic order parameter in fermionic determinant. Therefore we have studied the possibility of the phase transition to an excitonic phase by means of simplified Monte-Carlo process on the hexagonal lattice. We show that this phase, whic…
Magnetism in transition-metal compounds (TMCs) has traditionally been associated with spin degrees of freedom, because the orbital magnetic moments are typically largely quenched. On the other hand, magnetic order in 4f- and 5d-electron systems arises from spin and orbital moments that are rigidly tied together by the large intra-atomic spin-orbit coupling (SOC). Using inelastic neutron scattering on the archetypal 4d-electron Mott insulator Ca$_2$RuO$_4$, we report a novel form of excitonic magnetism in the intermediate-strength regime of the SOC. The magnetic order is characterized by ``soft…
We study the excitonic semimetal-insulator quantum phase transition in three-dimensional Dirac semimetal in which the fermion dispersion is strongly anisotropic. After solving the Dyson-Schwinger equation for the excitonic gap, we obtain a global phase diagram in the plane spanned by the parameter for Coulomb interaction strength and the parameter for fermion velocity anisotropy. We find that excitonic gap generation is promoted as the interaction becomes stronger, but is suppressed if the anisotropy increases. Applying our results to two realistic three-dimensional Dirac semimetals Na$_{3}$Bi…
The single-site dynamical mean-field approximation is used to solve a model of high-Tc cuprate superconductors which includes both d_{x^2-y^2} and d_{3z^2-r^2} orbitals on the Cu as well as the relevant oxygen states. Both T (with apical oxygen) and T' (without apical oxygen) crystal structures are considered. In both phases, inclusion of the d_{3z^2-r^2} orbital is found to broaden the range of stability of the charge transfer insulating phase. For equal charge transfer energies and interaction strengths, the T' phase is found to be less strongly correlated than the T phase. For both structur…
The nonlinear optical response of an excitonic insulator coupled to lattice degrees of freedom is shown to depend in strong and characteristic ways on whether the insulating behavior originates primarily from electron-electron or electron-lattice interactions. Linear response optical signatures of the massive phase mode and the amplitude (Higgs) mode are identified. Upon nonlinear excitation resonant to the phase mode, a new in-gap mode at twice the phase mode frequency is induced, leading to a huge second harmonic response. Excitation of in-gap phonon modes leads to different and much smaller…
The electronic properties of excitonic insulators have been examined precisely in recent years. Pictures of exciton condensation may be applied to the spin-state transition observed in perovskite cobalt oxides. We examine the crystal-field and magnetic-field dependences of spatial spin structures on the basis of the density matrix renormalization group method using an effective model for the one-dimensional two-orbital Hubbard model in strong-coupling limit. We find an excitonic insulating (EI) phase and a spin-state ordering (SSO) phase in the intermediate region between low-spin and high-spi…
Material systems with Dirac electrons on a bipartite planar lattice and possessing superconducting and excitonic interactions are investigated both in the half-filling and doped regimes at zero temperature. Excitonic pairing is the analog of chiral symmetry breaking of relativistic fermion theories and produces an insulating gap in the electronic spectrum. Condensed matter systems with such competing interactions display phenomena that are analogous to the onset of the chiral condensate and of color superconductivity in dense quark matter. Evaluation of the free-energy (effective potential) al…
We investigate the half-filled two-orbital Hubbard model with the crystalline electric field using dynamical mean-field theory combined with the continuous-time quantum Monte Carlo simulations. We systematically study how the interplay of the intra- and interorbital Coulomb interations together with the Hund coupling realizes the diagonal and off-diagonal ordered states. It is found that the antiferroorbital ordered state is realized in the Hubbard model, in addition to the antiferromagnetically ordered and excitonic states. The competition between the antiferroorbital ordered and excitonic st…
Graphite under high magnetic field exhibits consecutive metal-insulator (MI) transitions as well as re-entrant insulator-metal (IM) transition in the quasi-quantum limit at low temperature. In this paper, we identify the low-$T$ insulating phases as excitonic insulators with spin nematic orderings. We first point out that graphite under the relevant field regime is in the charge neutrality region, where electron and hole densities compensate each other. Based on this observation, we introduce interacting electron models with electron pocket(s) and hole pocket(s) and enumerate possible umklapp …
Excitonic insulator (EI) is an intriguing insulating phase of matter, where electrons and holes are bonded into pairs, so called excitons, and form a phase-coherent state via Bose-Einstein Condensation (BEC). Its theoretical concept has been proposed several decades ago, but the followed research is very limited, due to the rare occurrence of EI in natural materials and the lack of manipulating method of excitonic condensation. In this paper, we report the realization of a doping-controlled EI-to-semi-metal transition in Ta$_2$NiSe$_5$ using $in$-$situ$ potassium deposition. Combining with ang…
