Neutron scattering is a powerful tool to study magnetic structures and dynamics, benefiting from a precisely established theoretical framework. The neutron dipole moment interacts with electrons in materials via their magnetic field, which can have spin and orbital origins. Yet in most experimentally studied cases the individual degrees of freedom are well described within the dipole approximation, sometimes accompanied by further terms of a multipolar expansion that usually act as minor corrections to the dipole form factor. Here we report a unique example of neutrons diffracted mainly by magnetic octupoles. This unusual situation arises in a quantum spin ice where the electronic wavefunction becomes essentially octupolar under the effect of correlations. The discovery of such a new type of quantum spin liquid that comes with a specific experimental signature in neutron scattering is remarkable, because these topical states of matter are notoriously difficult to detect.
Spin liquids are highly correlated yet disordered states formed by the entanglement of magnetic dipoles$^1$. Theories typically define such states using gauge fields and deconfined quasiparticle excitations that emerge from a simple rule governing the local ground state of a frustrated magnet. For example, the '2-in-2-out' ice rule for dipole moments on a tetrahedron can lead to a quantum spin ice in rare-earth pyrochlores - a state described by a lattice gauge theory of quantum electrodynamics$^{2-4}$. However, f-electron ions often carry multipole degrees of freedom of higher rank than dipol…
All interpretations of extensive magnetic neutron scattering data in the cited paper are at fault [Phys. Rev. X 12, 021015]. For, the expressions for scattered intensities therein do not contain the cerium multipole whose likely contribution to the magnetic state of the pyrochlore is a principal goal of the published investigation. The Comment includes a brief look at essential corrections to the theory.
We have performed a single crystal neutron scattering experiment on Ce0.7La0.3B6 to investigate the order parameter of phase IV microscopically. Below the phase transition temperature 1.5 K of phase IV, weak but distinct superlattice reflections at the scattering vector (h/2,h/2,l/2) (h, l = odd number) have been observed by neutron scattering for the first time. The intensity of the superlattice reflections is stronger for high scattering vectors, which is quite different from the usual magnetic form factor of magnetic dipoles. This result directly evidences that the order parameter of phase …
Classical symmetry enriched topological orders and distinct monopole charges for dipole-octupole spin ices
International Center for Quantum Materials, Peking University（北京大学量子材料中心）；Tsung-Dao Lee Institute, Shanghai Jiao Tong University（上海交通大学李政道研究所）；Collaborative Innovation Center of Quantum Matter（量子物质协同创新中心）；The University of Hong Kong, Shenzhen Institute of Research and Innovation（香港大学深圳研究院）；Beijing Key Laboratory of Quantum Devices, Peking University（北京大学量子器件北京市重点实验室）
Symmetry plays a fundamental role in our understanding of both conventional symmetry breaking phases and the more exotic quantum and topological phases of matter. We explore the experimental signatures of symmetry enriched U(1) quantum spin liquids (QSLs) on the pyrochlore lattice. We point out that the Ce local moment of the newly discovered pyrochlore QSL candidate Ce$_2$Sn$_2$O$_7$, is a dipole-octupole doublet. The generic model for these unusual doublets supports two distinct symmetry enriched U(1) QSL ground states in the corresponding quantum spin ice regimes. These two U(1) QSLs are du…
Single Crystal Diffuse Neutron Scattering Study of the Dipole-Octupole Quantum Spin Ice Candidate Ce$_2$Zr$_2$O$_7$: No Apparent Octupolar Correlations Above $T = 0.05$ K
本研究通过单晶漫散射中子衍射测量与数值连接团簇计算，发现在 $T = 0.05$ K 时 Ce$_2$Zr$_2$O$_7$ 仅表现出偶极自旋冰关联，未观察到八极关联散射的证据。
Signatures of field-induced multi-color kagome spin liquids in the dipole-octupole pyrochlore $\mathrm{Ce_2Hf_2O_7}$
Université Paris-Saclay, CNRS, Laboratoire de Physique des Solides（巴黎萨克雷大学，法国国家科学研究中心，固体物理实验室）；The Institute for Solid State Physics, The University of Tokyo（东京大学固体物质研究所）；Institut für Theoretische Physik and Würzburg-Dresden Cluster of Excellence ctd.qmat, Technische Universität Dresden（德累斯顿工业大学理论物理研究所及维尔茨堡-德累斯顿卓越集群ctd.qmat）；Department of Physics, The University of Tennessee（田纳西大学物理系）；Institute for Advanced Study, Chengdu University（成都大学高等研究院）；Department of Physics and Astronomy, McMaster University（麦克马斯特大学物理与天文学系）；Brockhouse Institute for Materials Research, McMaster University（麦克马斯特大学布罗克豪斯材料研究所）；Département de Physique, Université（大学物理系）
In his comment [arXiv:2209.03235], S. W. Lovesey argues that our analysis of neutron scattering experiments performed on Ce$_2$Zr$_2$O$_7$ is invalid. Lovesey argues that we have not properly accounted for the higher-order multipolar contributions to the magnetic scattering and that our use of pseudospin-$1/2$ operators to describe the scattering is inappropriate. In this reply, we show that the multipolar corrections discussed by Lovesey only become significant at scattering wavevectors exceeding those accessed in our experiments. This in no way contradicts or undermines our work, which never…
Neutron scattering measurements on the pyrochlore magnet Ce$_2$Zr$_2$O$_7$ reveal an unusual crystal field splitting of its lowest $J$=5/2 multiplet, such that its ground state doublet is composed of m$_J$=$\pm$3/2, giving these doublets a dipole - octupole (DO) character with local Ising anisotropy. Its magnetic susceptibility shows weak antiferromagnetic correlations with $θ_{CW}$=-0.4(2)K, leading to a naive expectation of an All-In, All-Out ordered state at low temperatures. Instead our low energy inelastic neutron scattering measurements show a dynamic quantum spin ice state, with suppres…
Quantum spin liquid (QSL) is a disordered state of quantum-mechanically entangled spins commonly arising from frustrated magnetic dipolar interactions. However, QSL in some pyrochlore magnets can also come from frustrated magnetic octupolar interactions. Although the key signature for both dipolar and octupolar interaction-driven QSL is the presence of a spin excitation continuum (spinons) arising from the spin quantum number fractionalization, an external magnetic field-induced ferromagnetic order will transform the spinons into conventional spin waves in a dipolar QSL. By contrast, in an oct…
The Bragg diffraction of neutrons and x-rays are well-suited to the task of determining the distribution of magnetization in crystals. Applications of the two techniques proceed by contrasting observed intensities with intensities calculated with a specific model, and changing the model as need be to achieve satisfactory agreement. An all-in-all-out (AIAO) magnetic configuration of magnetic dipoles on a cubic face-centred lattice with networks of corner-sharing tetrahedra is often mentioned in the context of pyrochlore oxides, for example, but the corresponding neutron and x-ray diffraction pa…
We present an experimental study of the pyrochlore coumpound Nd2Zr2O7 by means of neutron scattering and magnetization measurements down to 90 mK. The Nd$^{3+}$ magnetic moments exhibit a strong local $\langle$111$\rangle$ Ising anisotropy together with a dipolar-octupolar nature, different from the standard Kramers-doublet studied so far. We show that, despite the positive Curie-Weiss temperature, \ndzr\ undergoes a transition around 285 mK towards an all-in$-$all-out antiferromagnetic state. We establish the $(H,T)$ phase diagram in the three directions of the applied field and reveal a meta…
The Kitaev model, characterized by bond-dependent Ising spin interactions among spin-orbit entangled dipole moments in Mott insulators, offered a new approach to quantum spin liquids. Motivated by another type of bond-dependent interaction among quadrupole moments in $5d^2$ Mott insulators, we provide a microscopic route to uncover the Kitaev multipolar liquid, featuring fractionalized excitations out of non-Kramers doublets carrying multipole moments. The key ingredient is the magnetic field that allows for bond-anisotropic quadrupole-octupole interactions via mixing with the excited triplet …
There is a growing interest in the $U(1)$ Coulomb liquid in both quantum materials in pyrochlore ice and cluster Mott insulators and cold atom systems. We explore a paired hardcore boson model on a pyrochlore lattice. This model is equivalent to the XYZ spin model that was proposed for rare-earth pyrochlores with "dipole-octupole" doublets. Since this model has no sign problem for quantum Monte Carlo (QMC) simulations in a large parameter regime, we carry out both analytical and QMC calculations. We find that the $U(1)$ Coulomb liquid is quite stable and spans a rather large portion of the pha…
We argue that neutron spectra in a short-range ordered Valence Bond state is dominated by two-spinon states localized in small spatial regions such as a pinwheel. These excitations lead to angle averaged dynamic structure factor that is spread over a wide frequency range up to about $2.5 J$, whereas its wavevector dependence at all frequencies remains very close to that of isolated dimers. These results are in excellent agreement with recent Neutron scattering data in the Herbertsmithite materials ZnCu$_3$(OH)$_6$Cl$_2$.
We report time-of-flight neutron scattering measurements of the magnetic spectrum of Tb3+ in Tb2Ti2O7. The data, which extend up to 120 meV and have calibrated intensity, enable us to consolidate and extend previous studies of the single-ion crystal field spectrum. We successfully refine a model for the crystal field potential in Tb2Ti2O7 without relying on data from other rare earth titanate pyrochlores, and we confirm that the ground state is a non-Kramers doublet with predominantly |+/-4> components. We compare the model critically with earlier models.
Elastic neutron scattering experiments performed in semi-conducting La(1-x)Ca(x)MnO3 single crystals (x=0.05, 0.08), reveal new features in the problem of electronic phase separation and metal insulator transition. Below TN, the observation of a broad magnetic modulation in the q-dependent scattering intensity, centered at nearly identical qm whatever the q direction, can be explained by a liquid-like spatial distribution of similar magnetic droplets. A semi-quantitative description of their magnetic state, diameter, and average distance, can be done using a two-phase model. Such a picture can…
Motivated by spin-wave continuum (SWC) observed in recent neutron scattering experiments in Herbertsmithite, we use Gutzwiller-projected wave functions to study dynamic spin structure factor $S(\mathbf{q},ω)$ of spin liquid states on the kagome lattice. Spin-1 excited states in spin liquids are represented by Gutzwiller-projected two-spinon excited wave functions. We investigate three different spin liquid candidates, spinon Fermi-surface spin liquid (FSL), Dirac spin liquid (DSL) and random-flux spin liquid (RSL). FSL and RSL have low energy peaks in $S(\mathbf{q},ω)$ at $K$ points in the ext…
We propose an exactly solvable model for $j_{\text{eff}}=\frac32$ local moments on the honeycomb lattice. Our construction is guided by a symmetry analysis and by the requirement of an exact solution in terms of a Majorana fermion representation for multipole operators. The main interaction in the model can be interpreted as a bond-dependent quadrupole-quadrupole interaction. When time reversal symmetry is explicitly broken, we obtain a gapped spin liquid with a single chiral Majorana edge mode. We also investigate another solvable model in which the time-reversal-invariant spin liquid is coup…
