Hidden multipolar orders in spin-orbit-coupled Mott insulators provide a promising setting for correlated quantum matter, yet their control and detection remain major challenges. Here, we demonstrate that circularly polarized light enables both the control and detection of hidden multipolar order in $4d^2/5d^2$ systems with edge-sharing octahedra. Using a Floquet Schrieffer-Wolff expansion of a driven Hubbard-Kanamori model, we derive a low-energy multipolar Hamiltonian with two qualitatively new light-driven terms. One is an effective static field that couples linearly to the magnetic octupole, realizing an octupolar inverse Faraday effect. The other is a bond-dependent anisotropic exchange interaction absent in equilibrium. These two couplings constitute the key mechanisms of this work: the first provides a direct optical handle on hidden octupolar order, while the second reorganizes the multipolar exchange landscape and introduces strong bond-dependent frustration. Together, these couplings define a nonequilibrium multipolar Hamiltonian whose phase diagram contains robust antiferro-octupolar, ferro-octupolar, and partially polarized ferro-quadrupolar phases, alongside a putative Ising-octupolar regime and a strongly frustrated, liquid-like multipolar regime whose finite-size numerical signatures are compatible with Kitaev-type behavior. We further show that the induced multipolar order couples to the lattice, generating reversible trigonal and orthorhombic or tetragonal distortions that provide symmetry-resolved structural fingerprints in pump-probe experiments. In this way, our work establishes a general mechanism for the optical generation, control, and detection of hidden multipolar quantum states.
Quantum magnets with spin $J=2$, which arise in spin-orbit coupled Mott insulators, can potentially display multipolar orders. We carry out an exact diagonalization study of a simple octahedral crystal field Hamiltonian for two electrons, incorporating spin-orbit coupling (SOC) and interactions, finding that either explicitly including the $e_g$ orbitals, or going beyond the rotationally invariant Coulomb interaction within the $t_{2g}$ sector, causes a degeneracy breaking of the $J\!=\!2$ level degeneracy. This can lead to a low-lying non-Kramers doublet carrying quadrupolar and octupolar mom…
In 5$d^2$ Mott insulators with strong spin-orbit coupling, the lowest pseudospin states form a non-Kramers doublet, which carries quadrupolar and octupolar moments. A family of double perovskites where magnetic ions form a face-centered cubic (fcc) lattice was suggested to unveil an octupolar order offering a rare example in $d$-orbital systems. The proposed order requires a ferromagnetic (FM) octupolar interaction, since the antiferromagnetic (AFM) Ising model is highly frustrated on the fcc lattice. A microscopic model was recently derived for various lattices: for an edge-sharing octahedra …
Exotic high-rank multipolar order parameters have been found to be unexpectedly active in more and more correlated materials in recent years. Such multipoles are usually dubbed as "Hidden Orders" since they are insensitive to common experimental probes. Theoretically, it is also difficult to predict multipolar orders via \textit{ab initio} calculations in real materials. Here, we present an efficient method to predict possible multipoles in materials based on linear response theory under random phase approximation. Using this method, we successfully predict two pure meta-stable magnetic octupo…
Motivated by the recent development in strong spin-orbit-coupled materials, we consider the dipole-octupole doublets on the triangular lattice. We propose the most general interaction between these unusual local moments. Due to the spin-orbit entanglement and the special form of its wavefunction, the dipole-octupole doublet has a rather peculiar property under the lattice symmetry operation. As a result, the interaction is highly anisotropic in the pseudospin space, but remarkably, is uniform spatially. We analyze the ground state properties of this generic model and emphasize the hidden multi…
Broken symmetries in solids involving higher order multipolar degrees of freedom are historically referred to as "hidden orders" due to the formidable task of detecting them with conventional probes. Examples of such hidden orders include spin-nematic order in quantum magnets, and quadrupolar or higher multipolar orders in various correlated quantum materials. In this work, we theoretically propose that the study of magnetostriction provides a powerful and novel tool to directly detect higher-order multipolar symmetry breaking $-$ such as the elusive octupolar order $-$ by examining its scalin…
A series of Pr(TM)$_2$X$_{20}$ (with TM=Ti,V,Rh,Ir and X=Al,Zn) Kondo materials, containing non-Kramers Pr$^{3+}$ $4f^2$ moments on a diamond lattice, have been shown to exhibit intertwined orders such as quadrupolar order and superconductivity. Motivated by these experiments, we propose and study a Landau theory of multipolar order to capture the phase diagram and its field dependence. In zero magnetic field, we show that different quadrupolar states, or the coexistence of quadrupolar and octupolar orderings, may lead to ground states with multiple broken symmetries. Upon heating, such states…
Notable non-Fermi liquid and quantum critical behaviors are observed in rare-earth metallic systems with non-Kramers local moments supporting a number of different multipolar moments. A prominent example is $\text{Pr(Ti,V)}_{2}\text{Al}_{20}$, where the non-Kramers doublet of the $\text{Pr}^{3+}$ ion allows quadrupolar and octupolar moments, but lacks a dipolar moment. Previous theoretical studies show that a single impurity Kondo problem with such an unusual local moment leads to novel non-Fermi liquid states. In this work, we investigate possible quantum critical behaviors arising from the c…
Hidden Magnetic Octupolar Order driven by Spin-Orbit coupling in KFeF$_3$
University of Warwick（华威大学）；Durham University（杜伦大学）；University of Edinburgh（爱丁堡大学）；European Synchrotron Radiation Facility（欧洲同步辐射装置）；Institut Laue-Langevin（朗之万研究所）
The invariant form of the hyperfine interaction between multipolar moments and the nuclear spin is derived, and applied to discuss possibilities to identify the antiferro-octupolar (AFO) moments by NMR experiments. The ordered phase of NpO$_{2}$ and the phase IV of Ce$_{1-x}$La$_{x}$B$_{6}$ are studied in detail. Recent $^{17}$O NMR for polycrystalline samples of NpO$_{2}$ are discussed theoretically from our formulation. The observed feature of the splitting of $^{17}$O NMR spectrum into a sharp line and a broad line, their intensity ratio, and the magnetic field dependence of the shift and o…
Polaron-driven switching of octupolar order in doped 5d$^2$ double perovskite
University of Vienna（维也纳大学）；CPHT, CNRS, École polytechnique, Institut Polytechnique de Paris（巴黎综合理工学院）；Collège de France, Université PSL（法兰西公学院）；Department of Physics and Astronomy ”Augusto Righi”, Alma Mater Studiorum - Università di Bologna（博洛尼亚大学）
d- and f-shells support a large number of local degrees of freedom: dipoles, quadrupoles, octupoles, hexadecapoles, etc. Usually, the ordering of any multipole component leaves the system sufficiently symmetrical to allow a second symmetry breaking transition. Assuming that a second continuous phase transition occurs, we classify the possibilities. We construct the symmetry group of the first ordered phase, and then re-classify the order parameters in the new symmetry. While this is straightforward for dipole or quadrupole order, it is less familiar for octupole order. We give a group theoreti…
Motivated by experimental and theoretical interest in realizing multipolar orders in $d$-orbital materials, we discuss the quantum magnetism of $J\!=\!2$ ions which can be realized in spin-orbit coupled oxides with $5d^2$ transition metal ions. Based on the crystal field environment, we argue for a splitting of the $J\!=\!2$ multiplet, leading to a low lying non-Kramers doublet which hosts quadrupolar and octupolar moments. We discuss a microscopic mechanism whereby the combined perturbative effects of orbital repulsion and antiferromagnetic Heisenberg spin interactions leads to ferro-octupola…
Owing to comparably strong spin-orbit coupling and Hubbard interaction, iridium based 227 pyrochlore oxides harbor a rich confluence of competing magnetic orders and emergent multipolar Weyl quasiparticles. Here we show that this family of materials is predominantly susceptible toward the nucleation of electronic noncoplanar all-in all-out (AIAO) and three-in one-out (3I1O) orders, respectively transforming under the singlet $A_{2u}$ and triplet $T_{1u}$ representations, supporting octupolar and dipolar Weyl fermions, and favored by strong on-site Hubbard and nearest-neighbor ferromagnetic int…
We report time-of-flight neutron spectroscopic and diffraction studies of the 5$d^2$ cubic double pervoskite magnets, Ba$_2$MOsO$_6$ ($M$ = Zn, Mg, Ca). These cubic materials are all described by antiferromagnetically-coupled 5$d^2$ Os$^{6+}$ ions decorating a face-centred cubic (FCC) lattice. They all exhibit thermodynamic anomalies consistent with phase transitions at a temperature $T^*$, and exhibit a gapped magnetic excitation spectrum with spectral weight concentrated at wavevectors typical of type I antiferromagnetic orders. While muon spin resonance experiments show clear evidence for t…
Multipolar interactions are derived in the orbitally degenerate Anderson lattice with a spherical Fermi surface and one conduction electron per unit cell of the simple cubic lattice. As the crystalline-electric-field (CEF) ground state of $f^1$ configuration, the four-fold degenerate $Γ_8$ is mainly studied. Intersite interactions up to a sufficiently distant pair are Fourier transformed to the wavenumber space. For the $Γ_8$ case, quadrupolar and octupolar interactions favor the staggered order with $\mib{q} = (1/2,1/2,1/2)$, while the dipolar interaction favors an incommensurate magnetic str…
Discovery of novel spin-orbital entangled quantum ground states paves an important avenue for controllable quantum materials via unique couplings to the lattice and other external perturbations. In this work, motivated by recent experiments on cubic heavy fermion materials with multipolar local moments, we theoretically investigate strongly-interacting spin-orbital entangled quantum ground states in multipolar quantum impurity systems. Here itinerant electrons are interacting with the local moments carrying quadrupolar and octupolar moments, in contrast to the conventional Kondo problem with d…
Recent experiments have discovered multipolar orders in a variety of $d$-orbital Mott insulators. Motivated by uncovering the exchange interactions which underlie octupolar order proposed in the osmate double perovskites, we study a two-site model using exact diagonalization on a five-orbital Hamiltonian, incorporating spin-orbit coupling (SOC) and interactions, and including both intra-orbital and inter-orbital hopping. Using an exact Schrieffer-Wolff transformation, we then extract an effective pseudospin Hamiltonian for the non-Kramers doublets, uncovering dominant ferrooctupolar coupling d…
We investigate with a microscopic model anharmonic K-cation oscillation observed by neutron experiments in beta-pyrochlore superconductor KOs2O6, which also shows a mysterious first-order structural transition at Tp=7.5 K. We have identified a set of microscopic model parameters that successfully reproduce the observed temperature dependence and the superconducting transition temperature. Considering changes in the parameters at Tp, we can explain puzzling experimental results about electron-phonon coupling and neutron data. Our analysis demonstrates that the first-order transition is multipol…
The multipolar Kondo problem, wherein the quantum impurity carries higher-rank multipolar moments, has seen recent theoretical and experimental interest due to proposals of novel non-Fermi liquid states and the availability of a variety of material platforms. The multipolar nature of local moments, in conjunction with constraining crystal field symmetries, leads to a vast array of possible interactions and resulting non-Fermi liquid ground states. Previous works on Kondo physics have typically focussed on impurities that have two degenerate internal states. In this work, inspired by recent exp…
The magnetic properties of the pyrochlore iridate material Eu$_2$Ir$_2$O$_7$ (5$d^5$) have been studied based on the first principle calculations, where the crystal field splitting $Δ$, spin-orbit coupling (SOC) $λ$ and Coulomb interaction $U$ within Ir 5$d$ orbitals are all playing significant roles. The ground state phase diagram has been obtained with respect to the strength of SOC and Coulomb interaction $U$, where a stable anti-ferromagnetic ground state with all-in/all-out (AIAO) spin structure has been found. Besides, another anti-ferromagnetic states with close energy to AIAO have also…
We review the cubic rare-earth boride series which displays diverse electronic states like localized 4f electron multiplets split by the crystal electric field (CEF), itinerant heavy-fermion quasiparticle bands of the Kondo lattice as well as gapped Kondo insulator or mixed-valent semiconductor states. Fairly exotic states may appear due to the 'hidden' order of multipoles carried by degenerate CEF multiplets, in addition to magnetic order present in many RB6 (R = rare earth) compounds. Most prominent are CeB6 and its La-diluted alloys which exhibit antiferro-quadrupolar and octupolar ordering…
In contrast to magnetic order formed by electrons' dipolar moments, ordering phenomena associated with higher-order multipoles (quadrupoles, octupoles, etc.) are more difficult to characterize because of the limited choice of experimental probes that can distinguish different multipolar moments. The heavy-fermion compound CeB6 and its La-diluted alloys are among the best-studied realizations of the long-range-ordered multipolar phases, often referred to as "hidden order". Previously the hidden order in phase II was identified as primary antiferroquadrupolar (AFQ) and field-induced octupolar (A…
Experiments in the recently discovered vanadium-based kagome metals have suggested that their charge-ordered state displays not only bond distortions, characteristic of a ``real" charge density-wave (rCDW), but also time-reversal symmetry-breaking, typical of loop currents described by an ``imaginary" charge density-wave (iCDW). Here, we combine density-functional theory, group-theory, and phenomenological modeling to investigate the complex charge-ordered states that arise from interactions between the low-energy van Hove singularities present in the electronic structure of $A$V$_3$Sb$_5$. We…
