Interplay of itinerant electrons and Ising moments in a hybrid honeycomb quantum magnet TmNi$_3$Al$_9$
H. Ge, C. J. Huang, Q. Zhang, N. Zhao, L. Wang, J. Yang, Y. Fu, L. Zhang, Z. M. Song, T. T. Li, F. Ding, J. B. Xu, Y. F. Zhang, X. Tong, S. M. Wang, J. W. Mei, … 展开作者
H. Ge, C. J. Huang, Q. Zhang, N. Zhao, L. Wang, J. Yang, Y. Fu, L. Zhang, Z. M. Song, T. T. Li, F. Ding, J. B. Xu, Y. F. Zhang, X. Tong, S. M. Wang, J. W. Mei, A. Podlesnyak, L. S. Wu, Gang Chen, J. M. Sheng
The interplay between itinerant electrons and local magnetic moments in quantum materials brings about rich and fascinating phenomena and stimulates various developments in the theoretical framework. In this work, thermodynamic, electric transport, and neutron diffraction measurements were performed on a newly synthesized honeycomb lattice magnet TmNi$_3$Al$_9$. Based on the experimental data, a magnetic field temperature phase diagram was constructed, exhibiting three essentially different magnetic regions. Below ${T_{\rm N}=2.97 \pm 0.02}\ \rm K$ Tm$^{3+}$ moments order antiferromagnetically in zero field. We found that the Tm$^{3+}$ ions form a pseudo-doublet ground state with the Ising-like moments lying normal to the two-dimensional honeycomb layers. Application of a magnetic field along the easy axis gradually suppresses the antiferromagnetic order in favor of an induced ferromagnetic state above the critical field ${B_c=0.92 \pm 0.05}\ \rm T$. In the vicinity of $B_c$, a strong enhancement of the quantum spin fluctuations was observed. The quantum Ising nature of the local moments and the coupling to itinerant electrons are discussed.
Topological spin textures, such as a skyrmion crystal, are a source of unusual physical phenomena owing to the interplay between magnetism and topology. Since physical phenomena depend on the topological property and the symmetry of underlying spin structures, the search for new topological spin textures and emergent phenomena is one of the challenges in condensed matter physics. In this letter, we theoretically explore new topological spin textures arising from the synergy between spin, charge, and sublattice degrees of freedom in an itinerant magnet. By performing simulated annealing for an …
Using a hybrid method based on fermionic diagonalization and classical Monte Carlo, we investigate the interplay between itinerant and localized spins, with competing double- and super-exchange interactions, on a honeycomb lattice. For moderate superexchange, a geometrically frustrated triangular lattice of hexagons forms spontaneously. For slightly larger superexchange a dimerized groundstate is stable that has macroscopic degeneracy. The presence of these states on a non-frustrated honeycomb lattice highlights a novel phenomenon in this itinerant electron system: emergent geometrical frustra…
We use x-ray spectroscopy at Ir L$_3$/L$_2$ absorption edge to study powder samples of the intercalated honeycomb magnet Ag$_3$LiIr$_2$O$_6$. Based on x-ray absorption and resonant inelastic x-ray scattering measurements, and exact diagonalization calculations including next-neighbour Ir-Ir electron hoping integrals, we argue that the intercalation of Ag atoms results in a nearly itinerant electronic structure with enhanced Ir-O hybridization. As a result of the departure from the local relativistic $j_{\rm eff}\! = \!1/2$ state, we find that the relative orbital contribution to the magnetic m…
An effective low-energy Hamiltonian of itinerant electrons for iridium oxide Na2IrO3 is derived by an ab initio downfolding scheme. The model is then reduced to an effective spin model on a honeycomb lattice by the strong coupling expansion. Here we show that the ab initio model contains spin-spin anisotropic exchange terms in addition to the extensively studied Kitaev and Heisenberg exchange interactions, and allows to describe the experimentally observed zigzag magnetic order, interpreted as the state stabilized by the antiferromagnetic coupling of the ferromagnetic chains. We clarify possib…
Motivated by systems that can be seen as composed of two frustrated sublattices combined into a less frustrated total lattice, we study the double-exchange model with nearest-neighbor (NN) and next--nearest-neighbor (NNN) couplings on the honeycomb lattice. When adding NN hopping and its resulting double exchange to the antiferromagnetic (AFM) Heisenberg coupling, the resulting phase diagram is quite different from that of purely Heisenberg-like magnetic models and strongly depends on electron filling. For half filling, patterns of AFM dimers dominate, where the effective electronic bands rema…
Quantum phase transitions in the Hubbard model on the honeycomb lattice are investigated in the variational cluster approximation. The critical interaction for the paramagnetic to antiferromagnetic phase transition is found to be in remarkable agreement with a recent large-scale quantum Monte Carlo simulation. Calculated staggered magnetization increases continuously with $U$ and thus we find the phase transition is of a second order. We also find that the semimetal-insulator transition occurs at infinitesimally small interaction and thus a paramagnetic insulating state appears in a wide inter…
We report on a member of the spin-disordered honeycomb lattice antiferromagnet in a quasi-one-dimensional cobaltate Ba_3Co_2O_6(CO_3)_0.7. Resistivity exhibits as semimetallic along the face-sharing CoO6 chains. Magnetic susceptibility shows strongly anisotropic Ising-spin character with the easy axis along the chain due to significant spin-orbit coupling and a trigonal crystal field. Nevertheless, ^135Ba NMR detects no indication of the long-range magnetic order down to 0.48 K. Marginally itinerant electrons possess large entropy and low-lying excitations with a Wilson ratio R_W = 116, which …
Quantum spin liquid involves fractionalized quasipariticles such as spinons and visons. They are expressed as itinerant Majorana fermions and $Z_2$ fluxes in the Kitaev model with bond-dependent exchange interactions on a honeycomb spin lattice. The observation has recently attracted attention for a candidate material $α$-RuCl$_3$, showing spin liquid behaviour induced by a magnetic field. Since the observable spin excitation is inherently composed of the two quasiparticles, which further admix each other by setting in the magnetic field as well as non-Kitaev interactions, their individual ide…
We report the electronic and magnetic behaviour of the frustrated triangular metallic antiferromagnet 2H-AgNiO2 in high magnetic fields (54 T) using thermodynamic and transport measurements. Here localized d electrons are arranged on an antiferromagnetic triangular lattice nested inside a honeycomb lattice with itinerant d electrons. When the magnetic field is along the easy axis we observe a cascade of field-induced transitions, attributed to the competition between easy-axis anisotropy, geometrical frustration and coupling of the localized and itinerant system. The quantum oscillations data …
We investigate the competition between the spin-orbit interaction of itinerant electrons and their Kondo coupling with local moments densely distributed on the honeycomb lattice. We find that the model at half-filling displays a quantum phase transition between topological and Kondo insulators at a nonzero Kondo coupling. In the Kondo-screened case, tuning the electron concentration can lead to a new topological insulator phase. The results suggest that the heavy-fermion phase diagram contains a new regime with a competition among topological, Kondo-coherent and magnetic states, and that the r…
The electronic ground state in many iridate materials is described by a complex wave-function in which spin and orbital angular momenta are entangled due to relativistic spin-orbit coupling (SOC). Such a localized electronic state carries an effective total angular momentum of $J_{eff}=1/2$. In materials with an edge-sharing octahedral crystal structure, such as the honeycomb iridates Li2IrO3 and Na2IrO3, these $J_{eff}=1/2$ moments are expected to be coupled through a special bond-dependent magnetic interaction, which is a necessary condition for the realization of a Kitaev quantum spin liqui…
We consider electrons on a honeycomb or triangular lattice doped to the saddle point of the bandstructure. We assume system parameters are such that spin density wave (SDW) order emerges below a temperature $T_N$ and investigate the nature of the SDW phase. We argue that at $T < T_N$ the system develops a uniaxial SDW phase whose ordering pattern breaks $O(3) \times Z_4$ symmetry and corresponds to an eight site unit cell with non-uniform spin moments on different sites. This state is a half-metal -- it preserves full original Fermi surface, but has gapless charged excitations in one spin bran…
A prominent feature of quantum spin liquids is fractionalization of the spin degree of freedom. Fractionalized excitations have their own dynamics in different energy scales, and hence, affect finite-temperature ($T$) properties in a peculiar manner even in the paramagnetic state harboring the quantum spin liquid state. We here present a comprehensive theoretical study of the spin dynamics in a wide $T$ range for the Kitaev model on a honeycomb lattice, whose ground state is such a quantum spin liquid. In this model, the fractionalization occurs to break up quantum spins into itinerant matter …
Finite-temperature ($T$) properties of a Kitaev model defined on a honeycomb lattice are investigated by a quantum Monte Carlo simulation, from the viewpoint of fractionalization of quantum $S=1/2$ spins into two types of Majorana fermions, itinerant and localized. In this system, the entropy is released successively at two well-separated $T$ scales, as a clear indication of the thermal fractionalization. We show that the high-$T$ crossover, which is driven by itinerant Majorana fermions, is closely related with the development of nearest-neighbor spin correlations. On the other hand, the low-…
Antiferromagnetic Order and Magnetic Frustration in the Honeycomb Heavy-Fermion System Ce(Pt$_{1-x}$Pd$_{x}$)$_6$Al$_3$: $^{27}$Al and $^{195}$Pt NMR Studies
In this paper, by considering the Hubbard model on a honeycomb lattice, we developed a theory for the intrinsic magnetic impurities (MIs) with the quasi-localized spin moments induced by the vacancies in graphene. Because the intrinsic MIs are characterized by the zero modes that are rthotropic to the itinerant electrons, their properties are much different from those of Anderson MIs with the well-localized spin moments.
Honeycomb Crystal in a Mass-Asymmetric Electron-Hole Bilayer
Fudan University（复旦大学）；Shanghai Artificial Intelligence Laboratory（上海人工智能实验室）；The Hong Kong University of Science and Technology（香港科技大学）；Beijing National Laboratory for Condensed Matter Physics（北京凝聚态物理国家研究中心）；Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所）；International Center for Quantum Materials, School of Physics, Peking University（北京大学物理学院量子材料科学与工程中心）；Hefei National Laboratory（合肥国家实验室）
Kitaev quantum spin liquid is a topological magnetic quantum state characterized by Majorana fermions of fractionalized spin excitations, which are identical to their own antiparticles. Here, we demonstrate emergence of Majorana fermions thermally fractionalized in the Kitaev honeycomb spin lattice α-RuCl3. The specific heat data unveil the characteristic two-stage release of magnetic entropy involving localized and itinerant Majorana fermions. The inelastic neutron scattering results further corroborate these two distinct fermions by exhibiting quasielastic excitations at low energies around …
The layered honeycomb lattice iridate Cu$_2$IrO$_3$ is the closest realization of the Kitaev quantum spin liquid, primarily due to the enhanced interlayer separation and nearly ideal honeycomb lattice. We report pressure-induced structural evolution of Cu$_2$IrO$_3$ by powder x-ray diffraction (PXRD) up to $\sim$17 GPa and Raman scattering measurements up to $\sim$25 GPa. A structural phase transition (monoclinic $C2/c \: \rightarrow$ triclinic $P\bar{1}$) is observed with a broad mixed phase pressure range ($\sim$4 to 15 GPa). The triclinic phase consists of heavily distorted honeycomb lattic…
This work shows that any $k$-local Hamiltonian of qubits can be obtained from a 4-state 'Ising' model with $k$-local diagonal interactions and a single-site transverse field -- giving a new theoretical and experimental handle on quantum matter. In particular, the classical Ising interactions can be determined by replacing each Pauli operator with a $4 \times 4$ diagonal matrix. Subsequently tuning a large transverse field projects out two of the four states, recovering the original qubit model, with qudit generalizations. This leads to striking correspondences, such as the spin-1/2 XY and Heis…
Quantum Monte Carlo simulations are used to study the magnetic and transport properties of the Hubbard Model, and its strong coupling Heisenberg limit, on a one-third depleted square lattice. This is the geometry occupied, after charge ordering, by the spin-$\frac{1}{2}$ Ni$^{1+}$ atoms in a single layer of the nickelate materials La$_4$Ni$_3$O$_8$ and (predicted) La$_3$Ni$_2$O$_6$. Our model is also a description of strained graphene, where a honeycomb lattice has bond strengths which are inequivalent. For the Heisenberg case, we determine the location of the quantum critical point (QCP) wher…
The honeycomb Kitaev spin model provides a quantum spin liquid in the ground state, where the spin excitations are fractionalized into itinerant and localized Majorana fermions; the former spectrum has a broad continuum ranging up to a high energy, while the latter has a sharp peak at a low energy. Despite tremendous efforts, it remains elusive to clearly identify these distinct Majorana excitations in experiments. Here we show their manifestation in the time evolution after quenching the magnetic field, by using the time-dependent Majorana mean-field theory for both the ferromagnetic and anti…
A spin-$\frac{1}{2}$ Kitaev sublattice interacting with a subsystem of spinless fermions is studied on a honeycomb lattice when the fermion band is half filled. The model Hamiltonian describes a topological Kondo lattice with the Kitaev interaction, it is solved exactly by reduction to free Majorana fermions in a static $\mathbb{Z}_2$ gauge field. An yet unsolved problem of a hybridization of fermions and local moments in the Kondo lattice at low temperatures is solved in the framework of the model proposed. The Kondo hybridization gap is opened and the system is fixed in insulator and spin in…
We have investigated the longitudinal thermal conductivity of $α$-RuCl$_{3}$, the magnetic state of which is considered to be proximate to a Kitaev honeycomb model, along with the spin susceptibility and magnetic specific heat. We found that the temperature dependence of the thermal conductivity exhibits an additional peak around 100 K, which is well above the phonon peak temperature ($\sim$ 50 K). The higher-temperature peak position is comparable to the temperature scale of the Kitaev couplings rather than the Néel temperatures below 15 K. The additional heat conduction was observed for all …
The exactly-solvable Kitaev model of two-dimensional honeycomb magnet leads to a quantum spin liquid (QSL) characterized by Majorana fermions, relevant for fault-tolerant topological quantum computations. In the high-field paramagnetic state of $α$-RuCl3, half-integer quantization of thermal Hall conductivity has been reported as a signature of edge current, but the bulk nature of this state remains elusive. Here, from high-resolution heat capacity measurements under in-plane field rotation, we find strongly angle-dependent low-energy excitations in bulk $α$-RuCl3. The excitation gap has a sex…
Fractionalized excitations are of considerable interest in recent condensed-matter physics. Fractionalization of the spin degrees of freedom into localized and itinerant Majorana fermions are predicted for the Kitaev spin liquid, an exactly solvable model with bond-dependent interactions on a two-dimensional honeycomb lattice. As function of temperature, theory predicts a characteristic two-peak structure of the heat capacity as fingerprint of these excitations. Here we report on detailed heat-capacity experiments as function of temperature and magnetic field in high-quality single crystals of…
We investigate the impact of two types of disorder, bond randomness and site dilution, on the spin dynamics in the Kitaev model on a honeycomb lattice. The ground state of this model is a canonical quantum spin liquid with spin fractionalization into two types of quasiparticles, itinerant Majorana fermions and localized fluxes. Using unbiased quantum Monte Carlo simulations, we calculate the temperature evolution of the dynamical spin structure factor, the magnetic susceptibility, and the NMR relaxation rate. In the dynamical spin structure factor, we find that the two types of disorder affect…
The quantum Hall effect (QHE) in two-dimensional (2D) electron gases, which is one of the most striking phenomena in condensed matter physics, involves the topologically protected dissipationless charge current flow along the edges of the sample. Integer or fractional electrical conductance are measured in units of $e^2/2π\hbar$, which is associated with edge currents of electrons or quasiparticles with fractional charges, respectively. Here we discover a novel type of quantization of the Hall effect in an insulating 2D quantum magnet. In $α$-RuCl$_3$ with dominant Kitaev interaction on 2D hon…
Angular Modulations in Magnetic Torque Induced by Phase Transitions in the Triangular Supersolid $2H$-AgNiO$_2$
University of Oxford（牛津大学）；Harvard John A. Paulson School of Engineering and Applied Sciences（哈佛大学约翰·A·保尔森工程与应用科学学院）；Florida State University（佛罗里达州立大学）；Max-Planck-Institut fur Festkörperforschung（马克斯·普朗克固体研究所）
