An excitonic magnet hosts a condensate of spin-triplet excitons composed of conduction-band electrons and valence-band holes, and may be described by the two-orbital Hubbard model. When the Hamiltonian has the nearest-neighbor interorbital hopping integrals with $d$-wave symmetry and the number of electrons is slightly away from half filling, the $\boldsymbol{k}$-space spin texture appears in the excitonic phase with a broken time-reversal symmetry. We then show that, applying electric field to this doped excitonic magnet along a particular direction, a pure spin current emerges along its orthogonal direction. We discuss possible experimental realization of this type of the pure spin current in actual materials.
The theory of doped excitonic insulators is reinvestigated in light of recent experiments on hexaborides. For the appropriate valley-degenerate X_3,X_3' band structure, ``intra-valley'' condensation is energetically favored. Ferromagnetism occurs upon doping due to the quenching of kinetic energy at the otherwise direct first-order excitonic insulator-metal transition. The phase diagram includes states of spatially inhomogeneous density and magnetization at low temperatures.
The theory of impurities in excitonic insulator is investigated in the light of the recent experiments on hexaborides. First, we study the bound state around the impurity and find that the bound state emerges when ${Re}Δ$ is positive. Second, we study the continuum state using Abrikosov-Gor'kov's approach. We find that the energy gap is reduced strongly when ${Im}Δ=0$. Finally, we solve Bogoliubov-de Gennes equations for excitonic insulator numerically. We get the results consistent with the analytic ones. We also find that incomplete ferromagnetism appears in doped triplet excitonic insulator…
A three-orbital model derived from the two-dimensional projection of the $ab$ $initio$ Hamiltonian for alkaline doped fullerene A$_3$C$_{60}$ with A=Cs,Rb,K is studied by a variational Monte Carlo method. We correctly reproduce the experimental isotropic s-wave superconductivity around the $ab$ $initio$ parameters. With narrowing the bandwidth, the transition to an insulator is also reproduced, where orbital symmetry is found to be spontaneously broken with emergence of an excitonic Mott insulator for two orbitals and an antiferromagnetic insulator nearly degenerate with a spin liquid for the …
We investigate the competition between the superconducting and the excitonic phases on Dirac electrons on a bipartite planar lattice. The conditions for the appearance of superconductivity or excitonic condensate are given by the minima of the free energy and our results are explained.
Nesting in a semimetal can lead to an excitonic insulator state with spontaneous coherence between conduction and valence bands and a gap for charged excitations. In this paper we present a theory of the ferromagnetic state that occurs when the density of electrons in the conduction band and holes in the valence band differ. We find an unexpectedly rich doping-field phase diagram and an unusual collective excitation spectrum that includes two gapless collective modes. We predict regions of doping and external field in which phase-separated condensates of electrons and holes with parallel spins…
Engineering excitonic metal-insulator transitions in ultra-thin doped copper sulfides
Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences（中国科学院上海高等研究院）；Hefei National Laboratory（合肥国家实验室）
Using the dynamical mean-field approximation we investigate formation of excitonic condensate in the two-band Hubbard model in the vicinity of the spin-state transition. With temperature and band filling as the control parameters we realize all symmetry allowed spin-triplet excitonic phases, some exhibiting a ferromagnetic polarization. While the transitions are first-order at low temperatures, at elevated temperatures continuous transitions are found that give rise to a multi-critical point. Rapid but continuous transition between ferromagnetic and non-magnetic excitonic phases allows switchi…
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…
Using a weak-coupling renormalization group formalism, we study competing ordered phases for repulsively interacting fermions on the bilayer honeycomb lattice away from half-filling, which is realized experimentally as doped bilayer graphene. As electrons are added to the system, excitonic order is suppressed, and unconventional superconductivity appears generically in its place. In general it is found that the maximum critical temperature for superconductivity appears directly adjacent to the dome of particle-hole order, illustrating the importance of fluctuations in these channels for the fo…
The bilayer Hubbard model with electron-hole doping is an ideal platform to study excitonic orders due to suppressed recombination via spatial separation of electrons and holes. However, suffering from the sign problem, previous quantum Monte Carlo studies could not arrive at an unequivocal conclusion regarding the presence of phases with clear signatures of excitonic condensation in bilayer Hubbard models. Here, we develop a determinant quantum Monte Carlo (DQMC) algorithm for the bilayer Hubbard model that is sign-problem-free for equal and opposite doping in the two layers, and study excito…
Using a controlled weak-coupling renormalization group approach, we establish the mechanism of unconventional superconductivity in the vicinity of spin or charge ordered excitonic states for the case of electrons on the Bernal stacked bilayer honeycomb lattice. With one electron per site this system exhibits nearly parabolically touching conduction and valence bands. Such a state is unstable towards a spontaneous symmetry breaking, and repulsive interactions favor excitonic order, such as a charge nematic and/or a layer antiferromagnet. We find that upon adding charge carriers to the system, t…
We investigate spin-triplet exciton condensation in the two-orbital Hubbard model close to half filling by means of dynamical mean-field theory. Employing an impurity solver that handles complex off-diagonal hybridization functions, we study the behavior of excitonic condensate in stoichiometric and doped systems subject to external magnetic field. We find a general tendency of the triplet order parameter to lay perpendicular with the applied field and identify exceptions from this rule. For solutions exhibiting k-odd spin textures, we discuss the Bloch theorem which, in the absence of spin-or…
A tight binding model is introduced to describe the strong interaction limit of excitonic ordering. At stoichiometry, the model reduces in the strong coupling limit to a pseudo-spin model with approximate U(4) symmetry. Excitonic order appears in the pseudo-spin model as in-plane pseudo-magnetism. The U(4) symmetry unifies all possible singlet and triplet order parameters describing such states. Super-exchange, Hunds-rule coupling, and other perturbations act as anisotropies splitting the U(4) manifold, ultimately stabilizing a paramagnetic triplet state. The tendency to ferromagnetism with do…
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…
Excitonic magnetism involving superpositions of singlet and triplet states is expected to arise for two holes in strongly correlated and spin-orbit coupled $t_{2g}$ orbitals. However, uncontested material examples for its realization are rare. Applying the Variational Cluster Approach to the square lattice, we find conventional spin antiferromagnetism combined with orbital order at weak and excitonic order at strong spin-orbit coupling. We address the specific example of Ca$_2$RuO$_4$ using ab-initio modeling and conclude it to realize excitonic magnetism despite its pronounced orbital polariz…
The competition between spin-orbit coupling $λ$ and electron-electron interaction $U$ leads to a plethora of novel states of matter, extensively studied in the context of $t_{2g}^4$ and $t_{2g}^5$ materials, such as ruthenates and iridates. Excitonic magnets -- the antiferromagnetic state of bounded electron-hole pairs -- is a prominent example of phenomena driven by those competing energy scales. Interestingly, recent theoretical studies predicted that excitonic magnets can be found in the ground-state of spin-orbit-coupled $t_{2g}^4$ Hubbard models. Here, we present a detailed computational …
The effects associated with interatomic hoppings of excitons and the excitonic Bose condensate formation in the strongly correlated spin crossover systems are considered in the framework of the effective Hamiltonian for the two-band Kanamori model. The appearance of antiferromagnetic ordering due to the exciton order is found even in the absence of interatomic exchange interaction. The spectrum of excitonic excitations is calculated at various points of the "temperature vs. crystal field" phase diagram. Outside the region of exciton ordering, the spectrum has a gap, which vanishes at the bound…
We use the LDA+U method to study the possibility of exciton condensation in perovskites of transition metals with $d^6$ electronic configuration such as LaCoO$_3$. For realistic interaction parameters we find several distinct solutions exhibiting spin-triplet exciton condensate, which gives rise to a local spin density distribution while the ordered moments are vanishingly small. Rhombohedral distortion from the ideal cubic structure suppresses the ordered state, contrary to the spin-orbit coupling which enhances the excitonic condensation energy. We explain the trends observed in the numerica…
The effects associated with exciton Bose condensate formation in strongly correlated spin crossover systems are considered within the effective Hamiltonian obtained from the two-orbital Hubbard-Kanamori model. The collective excitations spectrum at various points of the temperature-crystal field phase diagram is calculated. The role of the electron-phonon interaction is discussed. The exciton and magnetic order photoenhancement (induction) in strongly correlated spin crossover systems a new mechanism based on the cooperative effect of electron-phonon and interatomic exchange interactions and t…
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…
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…
The combination of strong spin-orbit coupling and correlations, e.g. in ruthenates and iridates, has been proposed as a means to realize quantum materials with nontrivial topological properties. We discuss here Mott insulators where onsite spin-orbit coupling favors a local $J_{\textrm{tot}}=0$ singlet ground state. We investigate excitations into a low-lying triplet, triplons, and find them to acquire nontrivial band topology in a magnetic field. We also comment on magnetic states resulting from triplon condensation, where we find, in addition to the same ordered phases known from the $J_{\te…
In Mott insulators with the t^4_{2g} electronic configuration such as of Re^{3+}, Ru^{4+}, Os^{4+}, and Ir^{5+} ions, spin-orbit coupling dictates a Van Vleck-type nonmagnetic ground state with angular momentum J=0, and the magnetic response is governed by gapped singlet-triplet excitations. We derive the exchange interactions between these excitons and study their collective behavior on different lattices. In perovskites, a conventional Bose condensation of excitons into a magnetic state is found, while an unexpected one-dimensional behavior supporting spin-liquid states emerges in honeycomb …
We study the charge and spin density distributions of excitonic insulator (EI) states in the tight-binding approximation. We first discuss the charge and spin densities of the EI states when the valence and conduction bands are composed of orthogonal orbitals in a single atom. We show that the anisotropic charge or spin density distribution occurs in a unit cell (or atom) and a higher rank electric or magnetic multipole moment becomes finite, indicating that the EI state corresponds to the multipole order. A full description of the multipole moments for the $s$, $p$, and $d$ orbitals is then g…
Electron-hole mixing-induced fine structure in alkaline earth hexaborides leads to lower energy (temperature) scales, and thus stronger tendency toward an excitonic instability, than in their doped counterparts (viz. Ca(1-x)La(x)B(6), x=0.005), which are high Curie temperature, small moment ferromagnets. Comparison of Fermi surfaces and spectral distributions with de Haas - van Alphen (dHvA), optical, transport, and tunneling data indicates that SrB6 remains a fermionic semimetal down to (at least) 5 K, rather than forming an excitonic condensate. For the doped system the Curie temperature is …
We study the orbital diamagnetic susceptibility in excitonic condensation phase using the meanfield approximation for a two-band model defined on a square lattice. We find that, in semiconductors, the excitonic condensation acquires a finite diamagnetic susceptibility due to spontaneous hybridization between the valence and the conduction bands, whereas in semimetals, the diamagnetic susceptibility in the normal phase is suppressed by the excitonic condensation. We also study the orbital diamagnetic and Pauli paramagnetic susceptibilities of Ta2NiSe5 using a two-dimensional three-band model an…
We investigate few- and many-body states in half-filled maximally symmetric topological insulator flat bands realized by two degenerate Landau levels which experience opposite magnetic fields. This serves as a toy model of flat bands in moiré materials in which valleys have Chern numbers $C= \pm 1$. We argue that although the spontaneously polarized Ising Chern magnet is a natural ground state for repulsive Coulomb interactions, it can be in reasonable energetic competition with correlated states which can be viewed as Laughlin states of excitons when short distance corrections to the interact…
Theoretical studies recently predicted the condensation of spin-orbit excitons at momentum $q$=$π$ in $t_{2g}^4$ spin-orbit coupled three-orbital Hubbard models at electronic density $n=4$. In parallel, experiments involving iridates with non-integer valence states for the Ir ions are starting to attract considerable attention. In this publication, using the density matrix renormalization group technique we present evidence for the existence of a novel excitonic condensate at $n=3.5$ in a one-dimensional Hubbard model with a degenerate $t_{2g}$ sector, when in the presence of spin-orbit coupli…
Excitonic insulators are insulating states formed by the coherent condensation of electron and hole pairs into BCS-like states. Isotropic spatial wave functions are commonly considered for excitonic condensates since the attractive interaction among the electrons and the holes in semiconductors usually leads to $s$-wave excitons. Here, we propose a new type of excitonic insulator that exhibits order parameter with $p+ip$ symmetry and is characterized by a chiral Chern number $C_\textrm{c}=1/2$. This state displays the parity anomaly, which results in two novel topological properties: fractiona…
We point out the universal presence of the excitonic superexchange in spin-orbit-coupled Mott insulators. It is observed that, the restriction to the lowest spin-orbit-entangled "$J$" states may sometimes be insufficient to characterize the microscopic physics, and the virtual excitonic processes via the upper "$J$" states provide an important correction to the superexchange. We illustrate this excitonic superexchange from a two-dimensional $5d$ iridate Sr$_2$IrO$_4$ and explain its physical consequences such as the orbital-like coupling to the external magnetic flux and the nonlinear magnetic…
We use the LDA+U approach to search for possible ordered ground states of LaSrCoO$_4$. We find a staggered arrangement of magnetic multipoles to be stable over a broad range of Co $3d$ interaction parameters. This ordered state can be described as a spin-denity-wave-type condensate of $d_{xy} \otimes d_{x^2-y^2}$ excitons carrying spin $S=1$. Further, we construct an effective strong-coupling model, calculate the exciton dispersion and investigate closing of the exciton gap, which marks the exciton condensation instability. Comparing the layered LaSrCoO$_4$ with its pseudo cubic analog LaCoO$_…
We present a dynamical mean-field study of dynamical susceptibilities in two-band Hubbard model. Varying the model parameters we analyze the two-particle excitations in the normal as well as in the ordered phase, an excitonic condensate. The two-particle DMFT spectra in the ordered phase reveal the gapless Goldstone modes arising from spontaneous breaking of continuous symmetries. We also observe gapped Higgs mode, characterized by vanishing of the gap at the phase boundary. Qualitative changes observed in the spin susceptibility can be used as an experimental probe to identify the excitonic c…
A superconducting (SC) state (Tc ~ 4.2K) has very recently been observed upon successful doping of the CDW ordered triangular lattice TiSe$_2$, with copper. Using high resolution photoemission spectroscopy we identify, for the first time, the momentum space locations of the doped electrons that form the Fermi sea of the parent superconductor. With doping, we find that the kinematic nesting volume increases whereas the coherence of the CDW order sharply drops. In the superconducting doping, we observe the emergence of a large density of states in the form of a narrow electron pocket near the \t…
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 present a general theory of multiorbital spin waves in magnetically ordered metallic systems. Motivated by the itinerant magnetism of iron-based superconductors, we compare the magnetic excitations for two different scenarios: when the magnetic order either sets in on the on-site orbital level; or when it appears as an electron-hole pairing between different bands of electron and hole character. As an example we treat the two-orbital model for iron-based superconductors. For small magnetic moments the spin excitations look similar in both scenarios. Going to larger interactions and larger m…
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 …
The electron-electron Coulomb interaction in Dirac-Weyl semimetals harbours a novel paradigm of correlation effects that hybridizes diverse realms of solid-state physics with their relativistic counterpart. Driving spontaneous mass acquisition, the excitonic condensate of strongly-interacting massless Dirac fermions is one such example whose exact nature remains debated. Here, by focussing on the two-dimensional tilted Dirac cones in the organic salt $α$-(BEDT-TTF)$_2$I$_3$, we show that the excitonic instability is controlled by a small chemicalpotential shift and an in-plane magnetic field. …
The condensation of spin-orbit-induced excitons in $(t_{2g})^4$ electronic systems is attracting considerable attention. In the large Hubbard U limit, antiferromagnetism was proposed to emerge from the Bose-Einstein Condensation (BEC) of triplons ($J_{\textrm{eff}} = 1$). In this publication, we show that even for the weak and intermediate U regimes, the spin-orbit exciton condensation is possible leading also to staggered magnetic order. The canonical electron-hole excitations (excitons) transform into local triplon excitations at large U , and this BEC strong coupling regime is smoothly conn…
We suggest that physics underlying the recently observed removal of sublattice and spin degeneracies in graphene in a strong magnetic field describes a phase transition connected with the generation of excitonic and spin gaps. The strong-coupling regime is described using a phenomenological model with enhanced Zeeman splitting (spin gap) and excitonic gaps. The experimental form of the Hall conductivity $σ_{xy}$ with the additional $ν= 0, \pm 1$ plateaus is reproduced. The form of $σ_{xy}$ in the case of a strong-coupling regime with no enhanced Zeeman splitting is also discussed.
Magnetic frustration can lead to peculiar magnetic orderings that break a discrete symmetry of the lattice in addition to the fundamental magnetic symmetries (i.e., spin rotation invariance and time-reversal symmetry). In this work, we focus on frustrated quantum magnets and study the nature of the quantum phase transition between a paramagnet and a magnetically ordered state with broken threefold ($Z_3$) crystal rotation symmetry. We predict the transition to happen in two stages, giving rise to an intermediate nematic phase in which rotation symmetry is broken but the system remains magnetic…
Manipulation of localized excitons in CrPS$_4$ by temperature and magnetic field
National University of Singapore（新加坡国立大学）；National Laboratory of the Rockies（落基山国家实验室）；Laboratoire National des Champs Magnétiques Intenses, LNCMI-EMFL, CNRS UPR3228,Univ. Grenoble Alpes, Univ. Toulouse, Univ. Toulouse 3, INSA-T（强磁场国家实验室，LNCMI-EMFL，CNRS UPR3228，格勒诺布尔阿尔卑斯大学，图卢兹大学，图卢兹第三大学，法国国家高等理工学院）；University of Chemistry and Technology Prague（布拉格化工大学）；King’s College London（伦敦国王学院）
We propose helicoidal excitonic phase in a Coulomb-coupled two-dimensional electron-hole double layer (EHDL) system with relativistic spin-orbit interaction. Previously, it was demonstrated that layered InAs/AlSb/GaInSb heterostructure is an ideal experimental platform for searching excitonic condensate phases, while its electron layer has non-negligible Rashba interaction. We clarify that due to the Rashba term, the spin-triplet (spin-1) exciton field in the EHDL system forms a helicoidal structure and the helicoid plane can be controlled by an in-plane Zeeman field. We show that due to small…
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 …
