We report a La2CuO4-like interlayer antiferromagnetic order in Sr2IrO4 films with large orthorhombic distortion (> 1.5%). The biaxial lattice strain in epitaxial heterostructures of Sr2IrO4/Ca3Ru2O7 lowers the crystal symmetry of Sr2IrO4 from tetragonal (C4) to orthorhombic (C2), guiding the Ir 5d Jeff = 1/2 pseudospin moment parallel to the elongated b-axis via magnetic anisotropy. From resonant X-ray scattering experiments, we observed an antiferromagnetic order in the orthorhombic Sr2IrO4 film whose interlayer stacking pattern is inverted from that of the tetragonal Sr2IrO4 crystal. This interlayer stacking is similar to that of the orthorhombic La2CuO4, implying that the asymmetric interlayer exchange interaction along a and b-directions exceeds the anisotropic interlayer pseudo-dipolar interaction. Our result suggests that strain-induced distortion can provide a delicate knob for tuning the long-range magnetic order in quasi-two-dimensional systems by evoking the competition between the interlayer exchange coupling and the pseudo-dipolar interaction.
We consider driving multi-orbital Mott insulators using laser radiation. We derive general expressions for periodically driven spin-orbital models using time-dependent perturbation theory in the strong interaction limit. We show that the effective exchange interactions of the Floquet spin-orbital Hamiltonian are highly tunable via variations of the frequency, amplitude, and polarization of the laser. We also take the effect of finite bandwidth of excitations into account and study possible heating effects. We further apply our formalism to orthorhombic titanates YTiO$_3$ and LaTiO$_3$ based on…
Mott state in 1T-TaS2 is predicted to host quantum spin liquids (QSL). However, its insulating mechanism is controversial due to complications from interlayer coupling. Here, we study the Mott state in monolayer 1T-NbSe2, an electronic analogy to TaS2 exempt from interlayer coupling, using spectroscopic imaging scanning tunneling microscopy and first principles calculations. Monolayer NbSe2 surprisingly displays two types of Star-of-David (SD) motifs with different Mott gap sizes, that are interconvertible via temperature variation. And, bilayer 1T-NbSe2 shows Mott collapse by interlayer coupl…
We study the electronic structure and magnetic interactions in methylamine-intercalated orthorhombic alkali-doped fullerene (CH3NH2)K3C60 within the density functional theory. As in the simpler ammonia intercalated compound (NH3)K3C60, the orthorhombic crystal-field anisotropy Δlifts the t1u triple degeneracy at the Γpoint and drives the system deep into the Mott-insulating phase. However, the computed Δand conduction electron bandwidth W cannot alone account for the abnormally low experimental Néel temperature, T_N = 11 K of the methylamine compound, compared to the much higher value T_N = 40…
High-quality Pr0.7Ca0.3MnO3/SrRuO3 superlattices were fabricated by pulsed laser deposition and were investigated by high-resolution transmission electron microscopy and SQUID magnetometry. Superlattices with orthorhombic and tetragonal SrRuO3 layers were investigated. The superlattices grew coherently; in the growth direction Pr0.7Ca0.3MnO3 layers were terminated by MnO2- and SrRuO3 layers by RuO2-planes. All superlattices showed antiferromagnetic interlayer coupling in low magnetic fields. The coupling strength was significantly higher for orthorhombic than for tetragonal symmetry of the SrR…
We have investigated the in-plane uniaxial pressure effect on the antiferromagnetic Mott insulator Ca2RuO4 from resistivity and magnetization measurements. We succeeded in inducing the ferromagnetic metallic phase at lower critical pressure than by hydrostatic pressure, indicating that the flattening distortion of the RuO6 octahedra is more easily released under in-plane uniaxial pressure. We also found a striking in-plane anisotropy in the pressure responses of various magnetic phases: Although the magnetization increases monotonically with pressure diagonal to the orthorhombic principal axes…
1T-TaS$_2$ undergoes successive phase transitions upon cooling and eventually enters an insulating state of mysterious origin. Some consider this state to be a band insulator with interlayer stacking order, yet others attribute it to Mott physics that support a quantum spin liquid state.Here, we determine the electronic and structural properties of 1T-TaS$_2$ using angle-resolved photoemission spectroscopy and X-Ray diffraction. At low temperatures, the 2$π$/2c-periodic band dispersion, along with half-integer-indexed diffraction peaks along the c axis, unambiguously indicates that the ground …
The consequences of the Jahn-Teller (JT) orbital-lattice coupling for magnetism of pseudospin J_{eff}=1/2 and J_{eff}=0 compounds are addressed. In the former case, represented by Sr_2IrO_4, this coupling generates, through the so-called pseudo-JT effect, orthorhombic deformations of a crystal concomitant with magnetic ordering. The orthorhombicity axis is tied to the magnetization and rotates with it under magnetic field. The theory resolves a number of puzzles in Sr_2IrO_4 such as the origin of in-plane magnetic anisotropy and magnon gaps, metamagnetic transition, etc. In J_{eff}=0 systems, …
Self-doped Molecular Mott Insulator for Bilayer High-Temperature Superconducting La3Ni2O7
Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所）；Kavli Institute for Theoretical Sciences, University of Chinese Academy of Sciences（中国科学院大学理论科学研究所）；School of Physical Sciences, University of Chinese Academy of Sciences（中国科学院大学物理科学学院）
We show that an interlayer exciton condensate doped into a strongly correlated Mott insulator exhibits a remarkable enhancement of the bandwidth of the magnetic excitations (triplons). This triplon is visible in the dynamical magnetic susceptibility and can be measured using resonant inelastic X-ray scattering. The bandwidth of the triplon scales with the exciton superfluid density, but only in the limit of strong correlations. As such the triplon bandwidth acts as a probe of exciton-spin interactions in the condensate.
Site-polarized Mott phases competing with a correlated metal in twisted WSe$_2$
University of Hamburg（汉堡大学）；The Hamburg Centre for Ultrafast Imaging（汉堡超快成像中心）；University of Würzburg（维尔茨堡大学）；Max Planck Institute for the Structure and Dynamics of Matter（物质结构与动力学马普研究所）；RWTH Aachen University（亚琛工业大学）；Center for Computational Quantum Physics, Flatiron Institute（平顿研究所计算量子物理中心）；Tsientang Institute for Advanced Study, Zhejiang（浙江大学前沿技术研究院（紫江））；Songshan Lake Materials Laboratory（松山湖材料实验室）
For continuous Mott metal-insulator transitions in layered two dimensional systems, we demonstrate the phenomenon of dimensional decoupling: the system behaves as a three-dimensional metal in the Fermi liquid side but as a stack of decoupled two-dimensional layers in the Mott insulator. We show that the dimensional decoupling happens at the Mott quantum critical point itself. We derive the temperature dependence of the interlayer electric conductivity in various crossover regimes near such a continuous Mott transition, and discuss experimental implications.
We theoretically investigate twisted structures where each layer is composed of a strongly correlated material. In particular, we study a twisted t-J model of cuprate multilayers within the slave-boson mean field theory. This treatment encompasses the Mott physics at small doping and self consistently generates d-wave pairing. Furthermore, including the correct inter-layer tunneling form factor consistent with the symmetry of the Cu $d_{x^2-y^2}$ orbital proves to be crucial for the phase diagram. We find spontaneous time reversal (T) breaking around twist angle of $45^\circ$, although only in…
The path from a Mott insulating phase to high temperature superconductivity encounters a rich set of unconventional phenomena involving the insulator-to-metal transition (IMT) such as emergent electronic orders and pseudogaps that ultimately affect the condensation of Cooper pairs. A huge hindrance to understanding the origin of these phenomena in the curates is the difficulty in accessing doping levels near the parent state. Recently, the J$_{eff}$=1/2 Mott state of the perovskite strontium iridates has revealed intriguing parallels to the cuprates, with the advantage that it provides unique …
We suggest that Cobalt-Oxychalcogenide layers constructed by vertex sharing CoA$_2$O$_2$ (A=S,Se,Te) tetrahedra, such as BaCoAO, are strongly correlated multi-orbital electron systems that can provide important clues on the cause of unconventional superconductivity. Differing from cuprates and iron-based superconductors, these systems lack of the C$_4$ rotational symmetry. However, their parental compounds possess antiferromagnetic(AFM) Mott insulating states through pure superexchange interactions and the low energy physics near Fermi surfaces upon doping is also attributed mainly to the thre…
The nearly free electron metal next to a localized Mott insulating state has been recently proposed as a way to probe Kondo lattice physics and to gain insight into how the two extremes of localized and delocalized electron states interact (Sunko, et al, Science advances 6, 2020). Although high harmonic generation has been used extensively to investigate the gas phase, its extension to solids is relatively recent, and has not yet been applied to interfaces. Here, we investigate the field-induced dielectric break-down at the Mott-insulator/metal interface using high harmonic generation, emitted…
We report an experimental investigation of the two-dimensional ${J}_{\rm eff}$ = 1/2 antiferromagnetic Mott insulator by varying the interlayer exchange coupling in [(SrIrO$_3$)$_1$, (SrTiO$_3$)$_m$] ($m$ = 1, 2 and 3) superlattices. Although all samples exhibited an insulating ground state with long-range magnetic order, temperature-dependent resistivity measurements showed a stronger insulating behavior in the $m$ = 2 and $m$ = 3 samples than the $m$ = 1 sample which displayed a clear kink at the magnetic transition. This difference indicates that the blocking effect of the excessive SrTiO$_…
We investigate the nature of the insulating phases in a bilayer Hubbard model with intralayer coupling $t$ and interlayer coupling $t_{\perp}$ at large interaction strength $U/t$ and half-filling. We consider a dynamical cluster approximation with a cluster size of $N_c=2\times4$, where short-range spatial fluctuations as well as on-site dynamical fluctuations are emphasized. By varying the band splitting ($t_{\perp}/t$), we find that at $t_{\perp}/t\simeq1.5$ the Mott behavior is rapidly suppressed in the momentum sectors ($π,0$) and ($0,π$). At $t_{\perp}/t\simeq2.5$ Mott features dominate i…
Charge separated interlayer excitons in transition metal dichalcogenide (TMDC) heterobilayers are being explored for moiré exciton lattices and exciton condensates. The presence of permanent dipole moments and the poorly screened Coulomb interaction make many body interactions particularly strong for interlayer excitons. Here we reveal two distinct phase transitions for interlayer excitons in the MoSe2/WSe2 heterobilayer using time and spatially resolved photoluminescence imaging: from trapped excitons in the moiré-potential to the modestly mobile exciton gas as exciton density increases to ne…
We demonstrate multiferroic behavior in trimerized Mott insulators through interplay between spins and electric dipole moments resulting from electronic charge fluctuations in frustrated units. The model consists of stacked triangular layers of trimers with small intertrimer exchange interactions $J'$ and $J"$. Ferroelectric states coexist with ferro- or antiferromagnetic orderings depending on the value of the magnetic field $H$ and the sign of the interlayer exchange $J"$. The electric polarization undergoes abrupt changes as a function of $H$.
We present ultra-high-resolution dilatometric studies in magnetic fields on a quasi-two-dimensional organic conductor $κ$-(D8-BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br, which is located close to the Mott metal-insulator (MI) transition. The obtained thermal expansion coefficient, $α(T)$, reveals two remarkable features: (i) the Mott MI transition temperature $T_{MI}$ = (13.6 $\pm$ 0.6)\,K is insensitive to fields up to 10\,T, the highest applied field; (ii) for fields along the interlayer \emph{b}-axis, a magnetic-field-induced (FI) phase transition at $T_{FI}$ = (9.5 $\pm$ 0.5)\,K is observed above a …
We study the electronic structure, magnetic state, and phase stability of paramagnetic BiNiO$_3$ near a pressure-induced Mott insulator-to-metal transition (MIT) by employing a combination of density functional and dynamical mean-field theory. We obtain that BiNiO$_3$ exhibits an anomalous negative-charge-transfer insulating state, characterized by charge disproportionation of the Bi $6s$ states, with Ni$^{2+}$ ions. Upon a compression of the lattice volume by $\sim$4.8\%, BiNiO$_3$ is found to make a Mott MIT, accompanied by the change of crystal structure from triclinic $P\bar{1}$ to orthorh…
Interlayer Coupling Driven Correlated and Charge-Ordered Electronic States in a Transition Metal Dichalcogenide Superlattice
Wuhan University（武汉大学）；Hubei University（湖北大学）；Hunan University（湖南大学）；ShanghaiTech University（上海科技大学）；University of Oxford（牛津大学）；Institute of Physics, Chinese Academy of Science（中国科学院物理研究所）；Nanjing University（南京大学）；Wuhan Institute of Quantum Technology（武汉量子技术研究院）
Candidates for correlated topological insulators, originated from the spin-orbit coupling as well as Hubbard type correlation, are expected in the ($111$) bilayer of perovskite-structural transition-metal oxides. Based on the first-principles calculation and tight-binding model, the electronic structure of a LaMnO$_3$ ($111$) bilayer sandwiched in LaScO$_3$ barriers has been investigated. For the ideal undistorted perovskite structure, the Fermi energy of LaMnO$_3$ ($111$) bilayer just stays at the Dirac point, rendering a semi-metal (graphene-like) which is also a half-metal (different from g…
The heat carriers responsible for the unexpectedly large thermal Hall conductivity of the cuprate Mott insulator La$_2$CuO$_4$ were recently shown to be phonons. However, the mechanism by which phonons in cuprates acquire chirality in a magnetic field is still unknown. Here, we report a similar thermal Hall conductivity in two cuprate Mott insulators with significantly different crystal structures and magnetic orders - Nd$_2$CuO$_4$ and Sr$_2$CuO$_2$Cl$_2$ - and show that two potential mechanisms can be excluded - the scattering of phonons by rare-earth impurities and by structural domains. Ou…
The Mott insulator YVO$_{3}$ with $T_{N}$ = 118 K is revisited to explore the role of spin, lattice and orbital correlations across the multiple structural and magnetic transitions observed as a function of temperature. Upon cooling, the crystal structure changes from orthorhombic to monoclinic at 200 K, and back to orthorhombic at 77 K, followed by magnetic transitions. From the paramagnetic high temperature phase, C-type ordering is first observed at 118 K, followed by a G-type spin re-orientation transition at 77 K. The dynamics of the transitions were investigated via inelastic neutron sca…
Combination of low-dimensionality and electron correlation is vital for exotic quantum phenomena such as the Mott-insulating phase and high-temperature superconductivity. Transition-metal dichalcogenide (TMD) 1T-TaS2 has evoked great interest owing to its unique nonmagnetic Mott-insulator nature coupled with a charge-density-wave (CDW). To functionalize such a complex phase, it is essential to enhance the CDW-Mott transition temperature TCDW-Mott, whereas this was difficult for bulk TMDs with TCDW-Mott < 200 K. Here we report a strong-coupling 2D CDW-Mott phase with a transition temperature on…
Ca2RuO4 is a structurally-driven Mott insulator with a metal-insulator transition at TMI = 357K, followed by a well-separated antiferromagnetic order at TN = 110 K. Slightly substituting Ru with a 3d transition metal ion M effectively shifts TMI by weakening the orthorhombic distortion and induces either metamagnetism or magnetization reversal below TN. Moreover, M doping for Ru produces negative thermal expansion in Ca2Ru1-xMxO4 (M = Cr, Mn, Fe or Cu); the lattice volume expands on cooling with a total volume expansion ratio, ΔV/V, reaching as high as 1%. The onset of the negative thermal exp…
Mott insulating behavior is induced by strong electron correlation and can lead to exotic states of matter such as unconventional superconductivity and quantum spin liquids. Recent advances in van der Waals material synthesis enable the exploration of novel Mott systems in the two-dimensional limit. Here we report characterization of the local electronic properties of single- and few-layer 1T-TaSe2 via spatial- and momentum-resolved spectroscopy involving scanning tunneling microscopy and angle-resolved photoemission. Our combined experimental and theoretical study indicates that electron corr…
We consider an efficient scheme to simulate fermionic Hubbard models with nonlocal density-density interactions in two dimensions, based on bond-centered auxiliary-field quantum Monte Carlo. The simulations are shown to be sign-problem free within a finite, restricted parameter range. Using this approach, we first study the Hubbard model on the half-filled square lattice bilayer, including an interlayer repulsion term in addition to the local repulsion, and present the ground state phase diagram within the accessible parameter region. Starting from the antiferromagnetically ordered state in th…
Dimensionality-Dependent Exciton Dispersion in a Single-Band Mott Insulator
Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所）；School of Physical Sciences, University of Chinese Academy of Sciences（中国科学院大学物理科学学院）；School of Physics, Zhejiang University（浙江大学物理学院）；State Key Laboratory of Silicon and Advanced Semiconductor Materials, Zhejiang University（浙江大学硅酸盐先进半导体材料国家重点实验室）；School of Physics and Beijing Key Laboratory of Opto-electronic Functional Materials & Micro-nano Devices, Renmin University of China（中国人民大学物理学院及光电功能材料与微纳器件北京市重点实验室）；Key Laboratory of Quantum State Construction and Manipulation (Ministry of Education), Renmin University of China（中国人民大学量子态构建与操控教育部重点实验室）；International Center for Quantum Materials, and Electron Microscopy Laboratory, School of Physics, Peking University（北京大学物理学院国际量子材料中心及电子显微镜实验室）；Department of Physics, Fuzhou University（福州大学物理系）
Layered transition metal dichalcogenide 1T-NbSe_2 is a good candidate to explore the charge density wave (CDW) and Mott physics. However, the effects of stacking orders and interlayer coupling in CDW 1T-NbSe_2 are still less explored and understood. Using density functional theory calculations, we present a systematic study of the electronic and magnetic properties of monolayer and layered CDW 1T-NbSe_2. Our results indicate that monolayer CDW 1T-NbSe_2 is a magnetic insulator with \sqrt13\times\sqrt13 periodic lattice modulation. Nevertheless, the magnetic properties of bilayer CDWs 1T-NbSe_2…
We investigate the dynamics of correlated charge carriers in the vicinity of the Mott metal-to-insulator transition in various of the title quasi-two-dimensional organic charge-transfer salts by means of fluctuation (noise) spectroscopy. The observed $1/f$-type fluctuations are quantitatively very well described by a phenomenological model based on the concept of non-exponetial kinetics. The main result is a correlation-induced enhancement of the fluctuations accompanied by a substantial shift of spectral weight to low frequencies close to the Mott critical endpoint. This sudden slowing down o…
We present first principles calculations of the electrostatic properties of Ba$_2$NaOsO$_6$ (BNOO), a 5$d^1$ Mott insulator with strong spin orbit coupling (SOC) in its low temperature quantum phases. In light of recent NMR experiments showing that BNOO develops a local octahedral distortion that is accompanied by the emergence of an electric field gradient (EFG) and precedes the formation of long range magnetic order [Lu et al., Nature Comm. 8, 14407 (2017), Liu et al., Phys. Rev. B. 97, 224103 (2018), Liu et al., Physica B. 536, 863 (2018)], we calculated BNOO's EFG tensor for several differ…
Local probe investigation of the spin dynamics in the kagome and inter-layers of orthorhombic barlowite Cu$_4$(OD)$_6$FBr: $^{79}$Br and $^{63}$Cu NQR study
Coupling together distinct correlated and topologically non-trivial electronic phases of matter can potentially induce novel electronic orders and phase transitions among them. Transition metal dichalcogenide compounds serve as a bedrock for exploration of such hybrid systems. They host a variety of exotic electronic phases and their Van der Waals nature enables to admix them, either by exfoliation and stacking or by stoichiometric growth, and thereby induce novel correlated complexes. Here we investigate the compound 4Hb-TaS$_2$ that interleaves the Mott-insulating state of 1T-TaS$_2$ and the…
We use quantum Monte Carlo simulations to study a dimer-diluted $S=1/2$ Heisenberg model on a bilayer square lattice with intralayer interaction $J_{1}$ and interlayer interaction $J_{2}$. Below the classical percolation threshold $p_c$, the system has three phases reachable by tuning the interaction ratio $g=J_{2}/J_{1}$: a N$\acute{e}$el ordered phase, a gapless quantum glass phase, and a gapped quantum paramagnetic phase. We present the ground-state phase diagram in the plane of dilution $p$ and interaction ratio $g$. The quantum glass phase is certified to be of the gapless Mott glass type…
Based on the density functional theory and our new model Hamiltonian, we have studied the basal-plane antiferromagnetism in the novel Jeff=1/2 Mott insulator Ba2IrO4. By comparing the magnetic properties of the bulk Ba2IrO4 with those of the single-layer Ba2IrO4, we demonstrate unambiguously that the basal-plane antiferromagnetism is caused by the intralyer magnetic interactions rather than by the previously proposed interlayer ones. In order to reveal the origin of the basal-plane antiferromagnetism, we propose a new model Hamiltonian by adding the single ion anisotropy and pseudo-quadrupole …
Using dynamical-mean-field theory for clusters, we study the two-dimensional Hubbard model in which electrons are coupled with the orthorhombic lattice distortions through the modulation in the hopping matrix. Instability towards spontaneous symmetry breaking from a tetragonal symmetric phase to an orthorhombic distorted phase is examined as a function of doping and interaction strength. A very strong instability is found in the underdoped pseudogap regime when the interaction strength is large enough to yield the Mott insulating phase at half filling. The symmetry breaking accompanies the rec…
