Mott insulators with localized magnetic moments will exhibit a quantum spin liquid state when the quantum fluctuations are strong enough to suppress the ordering of the spins. Such an entangled state will give rise to collective excitations, in which spin and charge information are carried separately. Our angle-resolved photoemission spectroscopy measurements on single-layer 1T-TaS_{2} show a flat band around the zone center and a gap opening of about 200 meV in the low temperature, indicating 2D Mott insulating nature in the system. This flat band is dispersionless in momentum space but shows anomalously broad width around the zone center and the spectral weight decays rapidly as momentum increases. The observation is described as a spectral continuum from electron fractionalization, corroborated by a low energy effective model. The intensity of the flat band is reduced by surface doping with magnetic adatoms and the gap is closing, a result from the interaction between spin impurities coupled with spinons and the chargons, which gives rise to a charge redistribution. Doping with nonmagnetic impurities behaves differently as the chemical potential shift dominates. These findings provide insight into the quantum spin liquid states of strongly correlated electrons on 2D triangular lattices.
Mott insulators with localized magnetic moments will exhibit a quantum spin liquid state when the quantum fluctuations are strong enough to suppress the ordering of the spins. Such an entangled state will give rise to collective excitations, in which spin and charge information are carried separately. Our angle-resolved photoemission spectroscopy measurements on single-layer 1T-TaS_{2} show a flat band around the zone center and a gap opening of about 200 meV in the low temperature, indicating 2D Mott insulating nature in the system. This flat band is dispersionless in momentum space but shows anomalously broad width around the zone center and the spectral weight decays rapidly as momentum increases. The observation is described as a spectral continuum from electron fractionalization, corroborated by a low energy effective model. The intensity of the flat band is reduced by surface doping with magnetic adatoms and the gap is closing, a result from the interaction between spin impurities coupled with spinons and the chargons, which gives rise to a charge redistribution. Doping with nonmagnetic impurities behaves differently as the chemical potential shift dominates. These findings provide insight into the quantum spin liquid states of strongly correlated electrons on 2D triangular lattices.
Effect of quenched disorder on a quantum spin liquid state of triangular-lattice antiferromagnet 1T-TaS2
A quantum spin liquid (QSL) is an exotic state of matter characterized by quantum entanglement and the absence of any broken symmetry. A long-standing open problem, which is a key for fundamental understanding the mysterious QSL states, is how the quantum fluctuations respond to randomness due to quenched disorder. Transition metal dichalcogenide 1T-TaS2 is a candidate material that hosts a QSL ground state with spin-1/2 on the two-dimensional perfect triangular lattice. Here, we performed systematic studies of low-temperature heat capacity and thermal conductivity on pure, Se-substituted and electron irradiated crystals of 1T-TaS2. In pure 1T-TaS2, the linear temperature term of the heat capacity γT and the finite residual linear term of the thermal conductivity in the zero-temperature limit κ0/T≡κ/T(T→0) are clearly resolved, consistent with the presence of gapless spinons with a Fermi surface. Moreover, while the strong magnetic field slightly enhances κ0/T, it strongly suppresses γ. These unusual contrasting responses to magnetic field imply the coexistence of two types of gapless excitations with itinerant and localized characters. Introduction of additional weak random exchange disorder in 1T-Ta(S1−xSex)2 leads to vanishing of κ0/T, indicating that the itinerant gapless excitations are sensitive to the disorder. On the other hand, in both pure and Se-substituted systems, the magnetic contribution of the heat capacity obeys a universal scaling relation, which is consistent with a theory that assumes the presence of localized orphan spins forming random singlets. Electron irradiation in pure 1T-TaS2 largely enhances γ and changes the scaling function dramatically, suggesting a possible new state of spin liquid.
Motivated by recent experiments on the quantum-spin-liquid candidate material LiZn2Mo3O8, we study a single-band extended Hubbard model on an anisotropic Kagome lattice with the 1/6 electron filling. Due to the partial filling of the lattice, the inter-site repulsive interaction is necessary to generate Mott insulators, where electrons are localized in clusters, rather than at lattice sites. We provide examples of such cluster Mott insulators and study the phase transitions between metallic states and cluster Mott insulators on an anisotropic Kagome lattice. It is shown that these cluster Mott insulators are generally U(1) quantum spin liquids with spinon Fermi surfaces. However, the nature of charge excitations in different cluster Mott insulators could be quite different and we show that there exists a novel cluster Mott insulator where charge fluctuations around the hexagonal cluster induce a plaquette charge order (PCO). The spinon excitation spectrum in this spin-liquid cluster Mott insulator is reconstructed due to the PCO so that only 1/3 of the total spinon excitations are magnetically active. The strong coupling limit of the same model is also analyzed via a Kugel-Khomskii-like model. Based on these results, we propose that the anomalous behavior of the finite-temperature spin-susceptibility in LiZn2Mo3O8 may be explained by finite-temperature properties of the cluster Mott insulator with the PCO as well as fractionalized spinon excitations. Existing and possible future experiments on LiZn2Mo3O8, and other Mo-based cluster magnets are discussed in light of these theoretical predictions.
We investigate the connection between doping-induced in-gap states and underlying spin excitations in Mott insulators by employing cluster perturbation theory on one-dimensional (1D) and quasi-1D Kitaev-Hubbard models. By manipulating Kitaev-like hopping terms ( 𝑡 ′ ) that selectively control spin anisotropies in the strong-coupling limit, we establish a direct correspondence between the kinetic dispersion of the in-gap states and the spin excitation spectra. Specifically, in the Z chain, in-gap states evolve from a gapless dispersion to a gapped flat band as the system transitions from the Heisenberg to the Ising model, exhibiting a gap scaling of 2 𝑡 ′ 2 / 𝑈 that matches the Ising spin gap. In the XY chain, the in-gap states split into a dispersive and a flat branch at the Kitaev limit, mirroring the Jordan-Wigner fermionic spectrum. For the two-leg ladder, we observe an emergent broad continuum of in-gap states that reflects the fractionalization of spin excitations, accompanied by a gap manifesting the presence of topological 𝑍 2 visons. Our results establish a robust correspondence between charge and spin dynamics in doped Mott insulators and demonstrate that in-gap states can serve as a probe of exotic quantum spin phenomena, including fractionalization and topological excitations, offering a new pathway to investigate spin liquids via spectroscopic probes of charge excitations.
In strongly correlated electron systems, the emergence of states in the Mott gap in the single-particle spectrum following the doping of the Mott insulator is a remarkable feature that cannot be explained in a conventional rigid-band picture. Here, based on an analysis of the quantum numbers and the overlaps of relevant states, as well as through a demonstration using the ladder and bilayer $t\text{\ensuremath{-}}J$ models, it is shown that in a continuous Mott transition due to hole doping, the magnetically excited states of the Mott insulator generally emerge in the electron-addition spectrum with the dispersion relation shifted by the Fermi momentum in the momentum region where the lower Hubbard band is not completely filled. This implies that the dispersion relation of a free-electron-like mode in the electron-addition spectrum eventually transforms into essentially the momentum-shifted magnetic dispersion relation of the Mott insulator, while its spectral weight gradually disappears toward the Mott transition. This feature reflects the spin-charge separation of the Mott insulator.
Electronic band structures usually remain unaffected by doping via a chemical-potential shift or by increasing the temperature in conventional band insulators. In contrast, it has been shown that those of Mott and Kondo insulators can be altered by doping or by increasing the temperature: electronic modes are induced within the band gap, exhibiting momentum-shifted magnetic dispersion relations from the band edges. Here, this study demonstrates that the underlying mechanism of the remarkable strong-correlation effects can be generalized to the emergence of electronic modes caused by various spin and charge perturbations, including magnetization of spin-gapped Mott and Kondo insulators. These emergent modes can alter the band structure if a macroscopic number of spins or charges are excited by the perturbations at a given moment. The origins and dispersion relations of these emergent modes, particularly why and how the dispersion relations depend on the momentum and energy of the perturbations, are elucidated by investigating the selection rules and using the Bethe ansatz and the effective theory for weak inter-unit-cell hopping. The validity and generality of the theoretical results across different models and spatial dimensions are verified by numerical calculations for the one- and two-dimensional Hubbard models, periodic Anderson models, Kondo lattice models, and ladder and bilayer Hubbard models. This study provides crucial insights into why and how spin and charge perturbations can alter the band structure in strongly correlated insulators, thereby paving the way for band-structure engineering in strong-correlation electronics, which enables previously unexplored functionalities by exploiting the unconventional characteristics revealed in this paper.
The complex interplay between charge and spin dynamics lies at the heart of strongly correlated quantum materials, and it is a fundamental topic in basic research with far-reaching technological perspectives. We explore in this paper the dynamics of holes in a single-band, extended t - J model where the background spins form a Z 2 quantum spin liquid. Using a field theory approach based on a parton construction, we show that while the electrons for most momenta fractionalize into uncorrelated charge-carrying holons and spin-carrying spinons as generally expected for a quantum spin liquid, the spinon-holon scattering cross section diverges for certain momenta, signaling strong correlations. By deriving an effective low-energy Hamiltonian describing this dynamics, we demonstrate that these divergences are due to the formation of long-lived spinon-holon bound states. Since the wave function of these bound states is localized over a few lattice sites, they correspond to well-defined fermions with the same charge and spin as the underlying electrons. We then show that quantum gas microscopy with atoms in optical lattices provides an excellent platform for verifying and probing the internal spatial structure of these emerging fermions. The fermions will furthermore show up as clear quasiparticle peaks in angle-resolved photoemission spectroscopy with an intensity determined by their internal structure. For a nonzero hole concentration, the fermions form hole pockets with qualitatively the same location, shape, and intensity variation in the Brillouin zone as the so-called Fermi arcs observed in the pseudogap phase. Such agreement is remarkable since the Fermi arcs arise from the delicate interplay between the symmetry of the quantum spin liquid and the internal structure of the emerging fermions in a minimal single-band model with no extra degrees of freedom added. Our results, therefore, provide a microscopic mechanism for the conjectured fractionalized Fermi liquid and open up new pathways for exploring the pseudogap phase and high-temperature superconductivity as arising from a quantum spin liquid.