α-RuCl3 is a Kitaev material suggested to be a proximate quantum spin liquid in a certain temperature and magnetic field range. Nonequilibrium measurements of transient dynamics have been proposed to detect fractionalized particles that emerge in the spin liquid and to possibly drive the system into novel photoinduced magnetic states that cannot be accessed by conventional equilibrium probes. Here we study ultrafast spin dynamics of photoinduced excitations in α-RuCl3 using pump-probe transient grating spectroscopy. In the real part of the complex transient reflectance change ΔR/R, we observe the long-range antiferromagnetic correlation near the Néel temperature. Most intriguingly, above the Néel temperature in the Kitaev paramagnetic phase, we reveal a photoexcitation component sensitive to the in-plane magnetic field in the imaginary part of ΔR/R. This component exhibits two distinct lifetimes of about tens of picoseconds. This photoexcitation component may be connected to novel photoexcited states in the Kitaev quantum spin liquid, and its lifetimes likely reflect the dynamics of unconventional spin excitations in the Kitaev model.
Quantum spin liquids are long-range entangled states of matter with emergent gauge fields and fractionalized excitations. While candidate materials, such as the Kitaev honeycomb ruthenate $α$-RuCl$_3$, show magnetic order at low temperatures $T$, here we demonstrate numerically a dynamical crossover from magnon-like behavior at low $T$ and frequencies $ω$ to long-lived fractionalized fermionic quasiparticles at higher $T$ and $ω$. This crossover is akin to the presence of spinon continua in quasi-1D spin chains. It is further shown to go hand in hand with persistent typicality down to very low…
In addition to the Kitaev ($K$) interaction, candidate Kitaev materials also possess Heisenberg ($J$) and off-diagonal symmetric ($Γ$) couplings. We investigate the quantum ($S = 1/2$) $K$-$J$-$Γ$ model on the honeycomb lattice by a variational Monte Carlo (VMC) method. In addition to the "generic" Kitaev spin liquid (KSL), we find that there is just one proximate KSL (PKSL) phase, while the rest of the phase diagram contains different magnetically ordered states. The PKSL is a gapless Z$_2$ state with 14 Majorana cones, which in contrast to the KSL has a gapless spin response. In a magnetic f…
We study the stability of Kitaev quasiparticles in the presence of a perturbing Heisenberg interaction as a Fock space localization phenomenon. We identify parameter regimes where Kitaev states are localized, fractal or delocalized in the Fock space of exact eigenstates, with the first two implying quasiparticle stability. Finite temperature calculations show that a vison gap, and a nonzero plaquette Wilson loop at low temperatures, both characteristic of the deconfined Kitaev spin liquid phase, persist far into the neighboring phase that has a concomitant stripy spin-density wave (SDW) order.…
Magnetic moments arranged at the corners of a honeycomb lattice are predicted to form a novel state of matter, Kitaev quantum spin liquid, under the influence of frustration effects between bond-dependent Ising interactions. Some layered honeycomb iridates and related materials, such as Na$_{2}$IrO$_{3}$ and $α$-RuCl$_{3}$, are proximate to Kitaev quantum spin liquid, but bosonic spin-wave excitations associated with undesirable antiferromagnetic long-range order mask the inherent properties of Kitaev Hamiltonian. Here, we use $^{63}$Cu nuclear quadrupole resonance to uncover the low energy sp…
Topological spin liquids in two spatial dimensions are stable phases in the presence of a small magnetic field, but may give way to field-induced phenomena at intermediate field strengths. Sandwiched between the low-field spin liquid physics and the high-field spin-polarized phase, the exploration of magnetic phenomena in this intermediate regime however often remains elusive to controlled analytical approaches. Here we numerically study such intermediate-field magnetic phenomena for two representative Kitaev models (on the square-octagon and decorated honeycomb lattice) that exhibit either Ab…
We perform a general study of spin ordering on the pyrochlore lattice with a 3:1 proportionality of two spin polarizations. Equivalently, this describes valence bond solid conformations of a quantum dimer model on the diamond lattice. We determine the set of likely low temperature ordered phases, on the assumption that the ordering is weak, i.e the system is close to a ``U(1)'' quantum spin liquid in which the 3:1 proportionality is maintained but the spins are strongly fluctuating. The nature of the 9 ordered states we find is determined by a ``projective symmetry'' analysis. All the phases e…
The Kitaev quantum spin liquid epitomizes an entangled topological state, for which two flavors of fractionalized low-energy excitations are predicted: the itinerant Majorana fermion and the Z2 gauge flux. Detection of these excitations remains challenging, because of their fractional quantum numbers and non-locality. It was proposed recently that fingerprints of fractional excitations are encoded in the phonon spectra of Kitaev quantum spin liquids through a novel fractional-excitation-phonon coupling. Here, we uncover this effect in $α$-RuCl3 using inelastic X-ray scattering with meV resolut…
Frustrated magnets with strong spin-orbit coupling promise to host topological states of matter, with fractionalized excitations and emergent gauge fields. Kitaev's proposal for a honeycomb-lattice Majorana spin liquid has triggered an intense search for experimental realizations, with bond-dependent Ising interaction being the essential building block. A prime candidate is $α$-RuCl$_3$ whose phase diagram in a magnetic field is, however, not understood to date. Here we present conclusive experimental evidence for a novel field-induced ordered phase in $α$-RuCl$_3$, sandwiched between the zigz…
The quasi two-dimensional Mott insulator $α$-RuCl$_3$ is proximate to the sought-after Kitaev quantum spin liquid (QSL). In a layer of $α$-RuCl$_3$ on graphene the dominant Kitaev exchange is further enhanced by strain. Recently, quantum oscillation (QO) measurements of such $α$-RuCl$_3$ / graphene heterostructures showed an anomalous temperature dependence beyond the standard Lifshitz-Kosevich (LK) description. Here, we develop a theory of anomalous QO in an effective Kitaev-Kondo lattice model in which the itinerant electrons of the graphene layer interact with the correlated magnetic layer …
Proximate quantum spin liquid state in the frustrated HoInCu$_4$ metal
Shiv Nadar Institution of Eminence（希夫纳德卓越学院）；PSI Center for Neutron and Muon Sciences CNM（瑞士保罗谢尔研究所中子与μ子科学中心）；Laboratorium für Festkörperphysik, ETH Zürich（苏黎世联邦理工学院凝聚态物理实验室）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理学研究所）；University of Augsburg（奥格斯堡大学）
The layered spiral magnet Cs2CuCl4 displays several interesting properties that have been suggested as evidence of proximity to a two dimensional quantum spin liquid. In this paper we study a concrete version of this proposal and suggest experiments that can potentially confirm it. We study universal critical properties of two-dimensional frustrated quantum magnets near the quantum phase transition between a spiral magnetic state and a spin liquid state with gapped bosonic spinons in the framework of the O(4) invariant critical theory proposed earlier(Chubukov et al, cond-mat/9402006). Direct …
$α$-RuCl$_{3}$ is a major candidate for the realization of the Kitaev quantum spin liquid, but its zigzag antiferromagnetic order at low temperatures indicates deviations from the Kitaev model. We have quantified the spin Hamiltonian of $α$-RuCl$_{3}$ by a resonant inelastic x-ray scattering study at the Ru $L_{3}$ absorption edge. In the paramagnetic state, the quasi-elastic intensity of magnetic excitations has a broad maximum around the zone center without any local maxima at the zigzag magnetic Bragg wavevectors. This finding implies that the zigzag order is fragile and readily destabilize…
We have investigated the field-angle behaviors of magnetic excitations under an in-plane magnetic field for proximate Kitaev systems. By employing the exact diagonalization method in conjunction with the linear spin wave theory, we have demonstrated that the magnetic excitation gap in the polarized phase is determined by the magnon excitation at $M$ points and has a strong anisotropy with respect to the field direction in the vicinity of the critical field limit. The specific heat from this magnon excitation bears qualitatively the same anisotropic behaviors as expected one for the non-Abelian…
Pyrochlore iridates and pyrochlore ices are two families of materials where novel quantum phenomena are intertwined with strong spin-orbit coupling, substantial electron correlation and geometrical frustration. Motivated by the puzzling experiments on two pyrochlore systems Pr2Ir2O7 and Yb2Ti2O7, we study the proximate Ising orders and the quantum phase transition out of quantum spin ice U(1) quantum spin liquid (QSL). We apply the electromagnetic duality of the compact quantum electrodynamics to analyze the "magnetic monopoles" condensation for U(1) QSL. The monopole condensation transition r…
Quantum matter provides an effective vacuum out of which arise emergent particles not corresponding to any experimentally detected elementary particle. Topological quantum materials in particular have become a focus of intense research in part because of the remarkable possibility to realize Majorana fermions, with their potential for new, decoherence-free quantum computing architectures. In this paper we undertake a study on high-quality single crystal of $α-RuCl_3$ which has been identified as a material realizing a proximate Kitaev state, a topological quantum state with magnetic Majorana f…
Given the parallelism between the physical properties of Ce and Yb based magnets and heavy fermions due to the electron-hole symmetry, it has been rather odd that the transition temperature of the Yb based compounds is normally very small, as low as $\sim$ 1 K or even lower, whereas Ce counterparts may often have the transition temperature well exceeding 10 K. Here, we report our experimental discovery of the transition temperature reaching 20 K for the first time in a Yb based compound at ambient pressure. The Mn substitution at the Al site in an intermediate valence state of $α$-YbAlB$_{4}$ …
Topological states of matter such as quantum spin liquids (QSLs) are of great interest because of their remarkable predicted properties including protection of quantum information and the emergence of Majorana fermions. Such QSLs, however, have proven difficult to identify experimentally. The most promising approach is to study their exotic nature via the wave-vector and intensity dependence of their dynamical response in neutron scattering. A major search has centered on iridate materials which are proposed to realize the celebrated Kitaev model on a honeycomb lattice - a prototypical topolog…
We introduce a matrix-product state based method to efficiently obtain dynamical response functions for two-dimensional microscopic Hamiltonians, which we apply to different phases of the Kitaev-Heisenberg model. We find significant broad high energy features beyond spin-wave theory even in the ordered phases proximate to spin liquids. This includes the phase with zig-zag order of the type observed in $α$-RuCl$_3$, where we find high energy features like those seen in inelastic neutron scattering experiments. Our results provide an example of a natural path for proximate spin liquid features t…
Proximate Spin Liquid Ground State Arising from Competing Stripy and 120$^{\circ}$ Spin Correlations in the Triangular Quantum Antiferromagnet ErMgGaO$_4$
In the quest for realizations of quantum spin liquids, the exploration of Kitaev materials - spin-orbit entangled Mott insulators with strong bond-directional exchanges - has taken center stage. However, in these materials the local spin-orbital j=1/2 moments typically show long-range magnetic order at low temperature, thus defying the formation of a spin-liquid ground state. Using resonant inelastic x-ray scattering (RIXS), we here report on a proximate spin liquid regime with clear fingerprints of Kitaev physics in the magnetic excitations of the honeycomb iridates alpha-Li2IrO3 and Na2IrO3.…
We identify fingerprints of a proximate quantum spin-liquid (QSL), observable by finite-temperature dynamical thermal transport within a minimal version of the idealized Kitaev model on a two-leg ladder, if subjected to inevitably present Heisenberg couplings. Using exact diagonalization and quantum typicality, we uncover (i) an insulator-conductor crossover induced by fracton recombination at infinitesimal Heisenberg coupling, (ii) low- and high-energy signatures of fractons, which survive far off the pure QSL point, and (iii) a non-monotonous current life-time versus Heisenberg couplings. Gu…
Excitation by light pulses enables the manipulation of phases of quantum condensed matter. Here, we photoexcite high-energy holon-doublon pairs as a way to alter the magnetic free energy landscape of the Kitaev-Heisenberg magnet $α$-RuCl$_3$, with the aim to dynamically stabilize a proximate spin liquid phase. The holon-doublon pair recombination through multimagnon emission is tracked through the time-evolution of the magnetic linear dichroism originating from the competing zigzag spin ordered ground state. A small holon-doublon density suffices to reach a spin disordered state. The phase tra…
We study the exchange interactions and resulting magnetic phases in the honeycomb cobaltates. For a broad range of trigonal crystal fields acting on Co2+ ions, the low-energy pseudospin-1/2 Hamiltonian is dominated by bond-dependent Ising couplings that constitute the Kitaev model. The non-Kitaev terms nearly vanish at small values of trigonal field Δ, resulting in spin liquid ground state. Considering Na3Co2SbO6 as an example, we find that this compound is proximate to a Kitaev spin liquid phase, and can be driven into it by slightly reducing Δby \sim 20 meV, e.g., via strain or pressure cont…
We report a comprehensive inelastic neutron-scattering study of the frustrated pyrochlore antiferromagnet MgCr2O4 in its cooperative paramagnetic regime. Theoretical modeling yields a microscopic Heisenberg model with exchange interactions up to third-nearest neighbors, which quantitatively explains all the details of the dynamic magnetic response. Our work demonstrates that the magnetic excitations in paramagnetic MgCr2O4 are faithfully represented in the entire Brillouin zone by a theory of magnons propagating in a highly-correlated paramagnetic background. Our results also suggest that MgCr…
We propose an unconventional topological quantum phase transition connecting a higher-order topological insulator (HOTI) and a featureless Mott insulator sharing the same symmetry patterns. We construct an effective theory description of the quantum critical point (QCP) by combining a bosonization approach and the coupled-stripe construction of 1D critical spin ladders. The phase transition theory is characterized by a critical dipole liquid theory with subsystem $U(1)$ symmetry whose low energy modes contain a Bose surface along the $k_x,k_y$ axis. Such a quantum critical point manifests frac…
Algebraic spin liquids, which are exotic gapless spin states preserving all microscopic symmetries, have been widely studied due to potential realizations in frustrated quantum magnets and the cuprates. At low energies, such putative phases are described by quantum electrodynamics in 2+1 dimensions. While significant progress has been made in understanding this nontrivial interacting field theory and the associated spin physics, one important issue which has proved elusive is the quantum numbers carried by so-called monopole operators. Here we address this issue in the ``staggered-flux'' spin …
We study the effect of Dzyaloshinskii-Moriya (DM) interaction on the triangular lattice $U(1)$ quantum spin liquid (QSL) which is stabilized by ring-exchange interactions. A weak DM interaction introduces a staggered flux to the $U(1)$ QSL state and changes the density of states at the spinon fermi surface. If the DM vector contains in-plane components, then the spinons gain nonzero Berry phase. The resultant thermal conductances $κ_{xx}$ and $κ_{xy}$ qualitatively agree with the experimental results on the material EtMe$_3$Sb[Pd(dmit)$_2]_2$. Furthermore, owing to perfect nesting of the fermi…
Although magnetically ordered at low temperatures, the spin-1/2 triangular antiferromagnet Cs_2CuCl_4 exhibits remarkable spin dynamics that strongly suggest proximity to a spin liquid phase. Here we address the question of whether a proximate spin liquid may also occur in an applied magnetic field, leaving a similar imprint on the dynamical spin correlations of this material. Specifically, we explore a spatially anisotropic Heisenberg spin-1/2 triangular antiferromagnet at 1/3 magnetization from a dual vortex perspective, and indeed find a new ``critical'' spin liquid phase described by QED3 …
Recent experiments suggest a quantum spin liquid ground state in the material PbCuTe$_2$O$_6$, where $S=1/2$ moments are coupled by antiferromagnetic Heisenberg interactions into a three dimensional structure of corner sharing triangles dubbed the hyper-hyperkagome lattice. It exhibits a richer connectivity, and thus likely a stronger geometric frustration, than the relatively well studied hyperkagome lattice. Here, we investigate the possible quantum spin liquids in the $S=1/2$ hyper-hyperkagome magnet using the complex fermion mean field theory. Extending the results of a previous projective…
We present an augmented parton mean-field theory which (i) reproduces the $exact$ ground state, spectrum, and dynamics of the quantum spin liquid phase of Kitaev's honeycomb model; and (ii) is amenable to the inclusion of integrability breaking terms, allowing a perturbation theory from a controlled starting point. Thus, we exemplarily study dynamical spin correlations of the honeycomb Kitaev quantum spin liquid within the $K-J-Γ$ model which includes Heisenberg and symmetric-anisotropic (pseudo-dipolar) interactions. This allows us to trace changes of the correlations in the regime of slowly …
We study the inelastic light scattering response in two- (2D) and three-dimensional (3D) Kitaev spin-liquid models with \ms band structures in the symmetry classes BDI and D leading to protected gapless surface modes. We present a detailed calculation of the resonant Raman/Brillouin scattering vertex relevant to iridate and ruthenate compounds whose low-energy physics is believed to be proximate to these spin-liquid phases. In the symmetry class BDI, we find that while the resonant scattering on thin films can detect the gapless boundary modes of spin liquids, the non-resonant processes do not…
Optical pump-probe experiments carried out in the time domain reveal both the intrinsic low energy dynamics and its connections to higher energy excitations in correlated electron systems. In this work, we propose two microscopic mechanisms for the optical generation of coherent magnetic modes in van der Waals magnets, and derive the corresponding effective light-spin interactions: either through pumping atomic orbital excitations resonantly or via a light-induced Floquet spin Hamiltonian, the ground state of the system is driven out of equilibrium. The subsequent long-time relaxational dynami…
Classification and correlation signatures of chiral spin liquids on the pyrochlore lattice
Université Paris-Saclay（巴黎萨克雷大学）；Kavli Institute for Theoretical Physics, University of California, Santa Barbara（加州大学圣塔芭芭拉分校卡弗里理论物理研究所）；Canadian Institute for Advanced Research（加拿大高级研究院）；Department of Physics, Indian Institute of Technology Madras（印度马德拉斯理工学院物理系）
We present a theoretical approach to describing the Mott transition of electrons on a two dimensional lattice that begins with the low energy effective theory of the Fermi liquid. The approach to the Mott transition must be characterized by the suppression of density and current fluctuations which correspond to specific shape deformations of the Fermi surface. We explore the nature of the Mott insulator and the corresponding Mott transition when these shape fluctuations of the Fermi surface are suppressed without making any a prior assumptions about other Fermi surface shape fluctuations. Buil…
Recently it was realized that the zigzag magnetic order in Kitaev materials can be stabilized by small negative off-diagonal interactions called the $Γ'$ terms. To fully understand the effect of the $Γ'$ interactions, we investigate the quantum $K$-$Γ$-$Γ'$ model on the honeycomb lattice using the variational Monte Carlo method. Two multinode Z$_2$ quantum spin liquids (QSLs) are found at $Γ'>0$, one of which is the previously found proximate Kitaev spin liquid called the PKSL14 state which shares the same projective symmetry group (PSG) with the Kitaev spin liquid. A remarkable result is that…
We develop a microscopic theory of the electronic nematic phase proximate to an isotropic Fermi liquid in both two and three dimensions. Explicit expressions are obtained for the small amplitude collective excitations in the ordered state; remarkably, the nematic Goldstone mode (the directorwave) is overdamped except along special directions dictated by symmetry. At the quantum critical point we find a dynamical exponent of $z=3$, implying stability of the gaussian fixed point. The leading perturbative effect of the overdamped Goldstone modes leads to a breakdown of Fermi liquid theory in the …
Recent interest in honeycomb lattice materials has focused on their potential to host quantum spin liquid (QSL) states. Variations in bond angles and spin allow a range of interesting behaviors on this lattice, from the predicted QSL ground state of the Kitaev model to exotic magnetic orders. Here we report the physical properties of two compounds with rare earths on an approximate honeycomb lattice. The isostructural compounds Nd$_2$S$_5$Sn (J = $\frac{9}{2}$) and Pr$_2$S$_5$Sn (J = 4) permit a direct comparison of half-integer versus integer spins on this lattice. We find strikingly differen…
Anomalous metals are observed in numerous experiments on disordered two-dimensional systems proximate to superconductivity. A characteristic feature of an anomalous metal is that its low temperature conductivity has a weakly temperature dependent value, significantly higher than that of a disordered Fermi liquid. We propose a dynamical mean-field model of an anomalous metal: interacting electrons similar in structure to that of the well-studied universal Hamiltonian of mesoscopic metallic grains, but with independent random interactions between pairs of sites, involving Cooper pair hopping and…
We describe the finite-size spectrum in the vicinity of the quantum critical point between a $\mathbb{Z}_2$ spin liquid and a coplanar antiferromagnet on the torus. We obtain the universal evolution of all low-lying states in an antiferromagnet with global SU(2) spin rotation symmetry, as it moves from the 4-fold topological degeneracy in a gapped $\mathbb{Z}_2$ spin liquid to the Anderson "tower-of-states" in the ordered antiferromagnet. Due to the existence of nontrivial order on either side of this transition, this critical point cannot be described in a conventional Landau-Ginzburg-Wilson …
Topologically ordered states of matter are generically characterized by excitations with quantum number fractionalization. A prime example is the spin liquid realized in Kitaev's honeycomb-lattice compass model where spin-flip excitations fractionalize into Majorana fermions and Ising gauge fluxes. While numerous compounds have been proposed to be proximate to such a spin-liquid phase, clear-cut evidence for fractionalized excitations is lacking. Here we employ microwave absorption measurements to study the low-energy excitations in $α$-RuCl$_3$ over a wide range of frequencies, magnetic field…
We report on terahertz spectroscopy of quantum spin dynamics in $α$-RuCl$_3$, a system proximate to the Kitaev honeycomb model, as a function of temperature and magnetic field. An extended magnetic continuum develops below the structural phase transition at $T_{s2}=62$K. With the onset of a long-range magnetic order at $T_N=6.5$K, spectral weight is transferred to a well-defined magnetic excitation at $\hbar ω_1 = 2.48$meV, which is accompanied by a higher-energy band at $\hbar ω_2 = 6.48$meV. Both excitations soften in magnetic field, signaling a quantum phase transition at $B_c=7$T where we …
We study spin S=1 and S=3/2 Heisenberg antiferromagnets on a cubic lattice focusing on spin solid states. Using Schwinger boson formulation for spins, we start in a U(1) spin liquid phase proximate to Neel phase and explore possible confining paramagnetic phases as we transition away from the spin liquid by the process of monopole condensation. Electromagnetic duality is used to rewrite the theory in terms of monopoles. For spin 1 we find several candidate phases of which the most natural one is a phase with spins organized into parallel Haldane chains. For spin 3/2 we find that the most natur…
