We uncover a high-field magnetic phase in i-MAX compounds exhibiting a canted antiferromagnetic (AFM) order with unprecedented properties, revealed through NMR and AC susceptibility. Intriguingly, as the atomic number of Rare Earth increases, the transition field of this canted AFM phase grows at the expense of the lower-field AFM state. Our findings point to the complexity of the magnetic structure in i-MAX compounds, demonstrating a non-trivial evolution of their phase diagram while increasing both the atomic number of the Rare Earth element and the external field.
The temperature-dependent evolution pattern of 5f electrons helps to elucidate the long-standing itinerant-localized dual nature in plutonium-based compounds. In this work, we investigate the correlated electronic states of PuIn3 dependence on temperature by using a combination of the density functional theory and the dynamical mean-field theory. Not only the experimental photoemission spectroscopy is correctly reproduced, but also a possible hidden 5f itinerant-localized crossover is identified. Moreover, it is found that the quasiparticle multiplets from the many-body transitions gradually e…
Since the discovery of charge disproportionation in the FeO$_2$ square-lattice compound Sr$_3$Fe$_2$O$_7$ by Mössbauer spectroscopy more than fifty years ago, the spatial ordering pattern of the disproportionated charges has remained "hidden" to conventional diffraction probes, despite numerous x-ray and neutron scattering studies. We have used neutron Larmor diffraction and Fe K-edge resonant x-ray scattering to demonstrate checkerboard charge order in the FeO$_2$ planes that vanishes at a sharp second-order phase transition upon heating above 332 K. Stacking disorder of the checkerboard patt…
Cerium hexaboride is a cubic f-electron heavy-fermion compound that displays a rich array of low-temperature magnetic ordering phenomena which have been the subject of investigation for more than 50 years. Its complex behaviour is the result of competing interactions, with both itinerant and local electrons playing important roles. Investigating this material has proven to be a substantial challenge, in particular because of the appearance of a "magnetically hidden order" phase, which remained elusive to neutron-scattering investigations for many years. It was not until the development of mode…
The temperature-dependent electronic structures of heavy fermion compound CeB$_{6}$ are investigated thoroughly by means of the combination of density functional theory and single-site dynamical mean-field theory. The band structure, density of states, and 4$f$ valence state fluctuation of CeB$_{6}$ are calculated in a broad temperature range of 10 $\sim$ 120 K. Overall, the 4$f$ electrons remain incoherent, approximately irrespective of the temperature. However, we find that these observables exhibit some unusual features near 20 K. In addition, the evolution of 4$f$ orbital occupancy, total …
We report on the first optical measurements of the rare-earth tri-telluride charge-density-wave systems. Our data, collected over an extremely broad spectral range, allow us to observe both the Drude component and the single-particle peak, ascribed to the contributions due to the free charge carriers and to the charge-density-wave gap excitation, respectively. The data analysis displays a diminishing impact of the charge-density-wave condensate on the electronic properties with decreasing lattice constant across the rare-earth series. We propose a possible mechanism describing this behavior an…
We performed the Shubnikov-de Haas (SdH) experiments of the low carrier heavy fermion compound URu2Si2 at high fields up to 34T and at low temperatures down to 30mK. All main SdH branches named alpha, beta and gamma were observed for all the measured field-directions (H // [001] -> [100], [100] -> [110] and [001] -> [110]), indicating that these are attributed to the closed Fermi surfaces with nearly spherical shapes. Anomalous split of branch alpha was detected for the field along the basal plane, and the split immediately disappears by tilting the field to [001] direction, implying a fingerp…
Using inelastic x-ray scattering beyond the dipole limit and hard x-ray photoelectron spectroscopy we establish the dual nature of the U $5f$ electrons in UM$_2$Si$_2$ (M = Pd, Ni, Ru, Fe), regardless of their degree of delocalization. We have observed that the compounds have in common a local atomic-like state that is well described by the U $5f^2$ configuration with the $Γ_1^{(1)}$ and $Γ_2$ quasi-doublet symmetry. The amount of the U 5$f^3$ configuration, however, varies considerably across the UM$_2$Si$_2$ series, indicating an increase of U5$f$ itineracy in going from M=Pd to Ni to Ru, an…
Layered 5$d$ transition iridium oxides, Sr$_2$(Ir,Rh)O$_4$, are described as unconventional Mott insulators with strong spin-orbit coupling. The undoped compound, Sr$_2$IrO$_4$, is a nearly ideal two-dimensional pseudospin-$1/2$ Heisenberg antiferromagnet, similarly to the insulating parent compound of high-temperature superconducting copper oxides. Using polarized neutron diffraction, we here report a hidden magnetic order in pure and doped Sr$_2$(Ir,Rh)O$_4$, distinct from the usual antiferromagnetic pseudo-spin ordering. We find that time-reversal symmetry is broken while the lattice transl…
A Heisenberg model over the square lattice recently introduced by Si and Abrahams to describe local-moment magnetism in the new class of Fe-As high-Tc superconductors is analyzed in the classical limit and on a small cluster by exact diagonalization. In the case of spin-1 iron atoms, large enough Heisenberg exchange interactions between neighboring spin-1/2 moments on different iron 3d orbitals that frustrate true magnetic order lead to hidden magnetic order that violates Hund's rule. It accounts for the low ordered magnetic moment observed by elastic neutron diffraction in an undoped parent c…
The heavy fermion compound URu$_2$Si$_2$ continues to attract great interest due to the unidentified hidden order it develops below 17.5K. The unique Ising character of the spin fluctuations and low temperature quasiparticles is well established. We present detailed measurements of the angular anisotropy of the nonlinear magnetization that reveal a $\cos^4 θ$ Ising anisotropy both at and above the ordering transition. With Landau theory, we show this implies a strongly Ising character of the itinerant hidden order parameter.
We report thermoelectric measurements of the low carrier heavy fermion compound URu2Si2 at high fields up to 34T and at low temperatures down to 500mK. The field dependence of the thermoelectric power (TEP) and the Nernst signal shows successive anomalies deep inside the hidden order (HO) phase. The field position of these anomalies correspond to different changes in the Shubnikov-de Haas frequencies and effective masses around 12 T, 17 T, 23 T and 30 T. These results indicate successive reconstructions of the Fermi surface, which imply electronic phase transitions well within the HO phase.
This Topical Review describes the multitude of unconventional behaviors in the hidden order, heavy fermion, antiferromagnetic and superconducting phases of the intermetallic compound URu$_2$Si$_2$ when tuned with pressure, magnetic field, and substitutions for all three elements. Such `perturbations' result in a variety of new phases beyond the mysterious hidden order that are only now being slowly understood through a series of state-of-the-science experimentation, along with an array of novel theoretical approaches. Despite all these efforts spanning more than 30 years, hidden order (HO) rem…
The heavy quasiparticle bands in Kondo materials which originate in the hybridization of f- and conduction electrons exhibit numerous, sometimes coexisting, broken symmetry phases. Most notable are unconventional superconductivity, itinerant small moment antiferromagnetism and hidden order of higher order multipoles of f-electrons which all lead to a gapping of the heavy bands. In rare cases the chemical potential lies within the hybridization gap and the ground state is a Kondo semiconductor without ordering. The dynamical magnetic response of such gapped f-electron systems has been investiga…
We have investigated the nature of the antiferromagnetic (AF) phase induced by uniaxial stress sigma in URu2Si2, by performing elastic neutron scattering measurements up to 0.4 GPa. We have found that the AF Bragg-peak intensity shows a clear hysteresis loop with sigma under the zero-stress cooling condition. The result strongly suggests that the sigma-induced AF phase is metastable and separated from the coexisting "hidden ordered" phase by a first-order phase transition. We also present the analyses of the crystalline strain effects, and suggest that the c/a ratio plays an important role in …
The static and dynamic magnetic properties of the Nd$_3$Ga$_5$SiO$_{14}$ compound, which appears as the first materialization of a rare-earth kagome-type lattice, were re-examined, owing to contradictory results in the previous studies. Neutron scattering, magnetization and specific heat measurements were performed and analyzed, in particular by fully taking account of the crystal electric field effects on the Nd$^{3+}$ ions. One of the novel findings is that the peculiar temperature independent spin dynamics observed below 10 K expresses single-ion quantum processes. This would short-circuit …
Laser driving in systems with competing or coupled electronic orders can lead to the enhancement of orders, or even to the appearance of hidden phases without an equilibrium analogue. Here we consider a model for A$_3$C$_{60}$ which exhibits a unique interplay between conventional and odd-frequency (or composite) orders. In particular, we show that photo-doping of the antiferromagnetic Mott insulating phase, as realized in Cs$_3$C$_{60}$, results in a paramagnetic gapped state with broken orbital symmetry. This hidden phase, which does not exist under equilibrium conditions, can be interpreted…
We use neutron scattering to compare the magnetic excitations in the hidden order (HO) and antiferromagnetic (AFM) phases in URu2-xFexSi2 as a function of Fe concentration. The magnetic excitation spectra change significantly between x = 0.05 and x = 0.10, following the enhancement of the AFM ordered moment, in good analogy to the behavior of the parent compound under applied pressure. Prominent lattice-commensurate low-energy excitations characteristic of the HO phase vanish in the AFM phase. The magnetic scattering is dominated by strong excitations along the Brillouin zone edges, underscori…
We present a first-principles many-body analysis of multi-orbital lattice susceptibilities in the metallic phase of the quasi-twodimensional compound LiVS$_2$. We base this on advanced correlated electronic structure methods for the $t_{2g}$-shell to reveal a highly entangled spin-orbital hexagonal ordering (SOHO) bringing about an inherently intersite order parameter for the trimerization transition, which eventually leads to an intriguing insulating phase at low temperature.
Spontaneous, collective ordering of electronic degrees of freedom leads to second-order phase transitions that are characterized by an order parameter. The notion "hidden order" (HO) has recently been used for a variety of materials where a clear phase transition occurs to a phase without a known order parameter. The prototype example is the heavy-fermion compound URu2Si2 where a mysterious HO transition occurs at 17.5K. For more than twenty years this system has been studied theoretically and experimentally without a firm grasp of the underlying physics. Using state-of-the-art density-functio…
The heavy-fermion compound URu2Si2 exhibits a hidden-order phase below the temperature, ~ 17.5 K. In spite of intense research for past three decades, no consensus on the order parameter exists and the nature has posed a long-standing mystery. Here we report the discovery of a Griffiths phase within the hidden-order phase, characterized by residual short-range correlations on the collapse of long-range orders due to the dilution effects. In the Griffiths phase scenario, strong evidence are provided for those cluster-like spins, such as the unique power-law behavior of magnetic susceptibility a…
We have investigated the influence of 3d-4f spin interaction on magnetic and magnetocaloric properties of DyCrO$_4$ and HoCrO$_4$ compounds by magnetization and heat capacity measurements. Both the compounds exhibit complicated magnetic properties and huge magnetic entropy change around the ferromagnetic transition due to the strong competition between ferromagnetic and antiferromagnetic superexchange interactions. For a field change of 8 T, the maximum values of magnetic entropy change ($ΔS_{M}^{max}$), adiabatic temperature change ($ΔT_{ad}$), and refrigerant capacity (RC) reach 29 J kg$^{-1…
We present a study of Nernst and Seebeck coefficients in the heavy-fermion compound URu$_{2}$Si$_{2}$, which hosts a phase transition of unsettled origin. A giant Nernst signal of unprecedented magnitude was found to emerge in the ordered state. Moreover, our analysis of the Seebeck and Hall data indicates that the ordering leads to a sudden increase in the entropy per itinerant electron and to a drastic decrease in the scattering rate.
Systematic analysis of the planar resistivity, Hall effect and cotangent of the Hall angle for the electron-doped cuprates reveals underlying Fermi-liquid behavior even deep in the antiferromagnetic part of the phase diagram. The transport scattering rate exhibits a quadratic temperature dependence, and is nearly independent of doping, compound and carrier type (electrons vs. holes), and hence universal. Our analysis moreover indicates that the material-specific resistivity upturn at low temperatures and low doping has the same origin in both electron- and hole-doped cuprates.
We have performed ultrasonic measurements on single-crystalline URu2Si2 with pulsed magnetic fields, in order to check for possible lattice instabilities due to the hybridized state and the hidden-order state of this compound. The elastic constant (C11-C12)/2, which is associated with a response to the Γ3-type symmetry-breaking (orthorhombic) strain field, shows a three-step increase at H > 35 T for H || c at low temperatures, where successive meta-magnetic transitions are observed in the magnetization. We discovered a new fact that the absolute change of the softening of (C11-C12)/2 in the te…
We have carried out a careful magnetic neutron scattering study of the heavy fermion compound \URuSi\ to probe the possible existence of a small magnetic moment parallel to tetragonal basal plane in the "hidden-order" phase. This small in-plane component of the magnetic moment on the uranium sites $S_\parallel$ has been postulated by two recent models (rank-5 superspin/hastatic order) aiming to explain the hidden-order phase, in addition to the well-known out-of-plane component $S_\perp ~ \approx~0.01-0.04 $μ_B$/U. In order to separate $S_\parallel$ and $S_\perp$ we take advantage of the condi…
We propose the magnetic exciton mediated superconductivity occurring in the enigmatic hidden-order phase of URu2Si2. The characteristic of the massive collective excitation observed only in the hidden-order phase is well reproduced by the antiferro hexadecapole ordering model as the trace of the dispersive crystalline-electric-field excitation. The disappearance of the superconductivity in the high-pressure antiferro magnetic phase can naturally be understood by the sudden suppression of the magnetic-exciton intensity. The analysis of the momentum dependence of the magnetic-exciton mode leads …
URu$_2$Si$_2$ is surely one of the most mysterious of the heavy-fermion compounds. Despite more than twenty years of experimental and theoretical works, the order parameter of the transition at $T_0 = 17.5$ K is still unknown. The state below $T_0$ remains called "hidden-order phase" and the stakes are still to identify the energy scales driving the system to this phase. We present new magnetoresistivity and magnetization measurements performed on very-high-quality single crystals in pulsed magnetic fields up to 60 T. We show that the transition to the hidden-order state in URu$_2$Si$_2$ is in…
We measured the magnetic susceptibilities of Cu$_6$Ge$_6$O$_{18}$-xH$_2$O ($x = 0 \sim 6$). Susceptibility above the antiferromagnetic (AF) transition temperature ($T_{\rm N}$) agrees with susceptibility of the one-dimensional Heisenberg $S = 1/2$ model with competing AF interactions. From the estimated ratio between nearest-neighbor and next-nearest-neighbor AF exchange interactions, the spin system is probably located near a boundary between spin systems with gapless and gapped magnetic excitation. The value of $T_{\rm N}/T_{\rm max}$, where $T_{\rm max}$ is temperature at which the suscepti…
We demonstrate that the volume of the Fermi surface, measured very precisely using de Haas-van Alphen oscillations, can be used to probe changes in the nature and occupancy of localized electronic states. In systems with unconventional ordered states, this allows an underlying electronic order parameter to be followed to very low temperatures. We describe this effect in the field-induced antiferroquadrupolar (AFQ) ordered phase of PrOs4Sb12, a heavy fermion intermetallic compound. We find that the phase of de Haas-van Alphen oscillations is sensitively coupled, through the Fermi volume, to the…
We report extensive muon spin rotation measurements on the lightly doped Y1-xCaxBa2Cu3O6+y compound, which allows us to disentangle the effect of disorder, controlled by random Ca2+ substitution, from that of mere doping. A 3D phase diagram of lightly doped cuprates is accurately drawn, showing that a thermally activated antiferromagnetic phase competes with superconductivity around a quantum critical point, hidden underneath a frozen insulating magnetic state. Disorder suppresses both competing order parameters and unveils the underlying frozen state. Doping and disorder destroy the activated…
Despite more than half a century of studies in heavy-fermion compounds, a full understanding of the various possible magnetic ordering phenomena is still far from complete. Some heavy-fermion materials show so-called hidden-order phases, which are invisible to conventional diffraction techniques. The multipolar moments of the $f$-electrons in their specific crystal field environment play a decisive role in the formation of these phases. Such hidden-order phases have been observed in a variety of compounds containing $4f$ and $5f$ elements, like URu$_2$Si$_2$, NpO$_2$, YbRu$_2$Ge$_2$, and CeB$_…
We present a comprehensive set of elastic and inelastic neutron scattering measurements on a range of Fe-doped samples of U(Ru$_{1-x}$Fe$_x$)$_2$Si$_2$ with 0.01~$\le~x~\le$~0.15. All of the samples measured exhibit long-range antiferromagnetic order, with the size of the magnetic moment quickly increasing to 0.51~$μ_B$ at 2.5\% doping and continuing to increase monotonically with doping, reaching 0.69~$μ_B$ at 15\% doping. Time-of-flight and inelastic triple-axis measurements show the existence of excitations at (1~0~0) and (1.4~0~0) in all samples, which are also observed in the parent compo…
A second-order phase transition is characterized by spontaneous symmetry breaking. The nature of the broken symmetry in the so-called "hidden order" phase transition in the heavy fermion compound URu2Si2, at transition temperature T_h=17.5 K, has posed a long-standing mystery. We report the emergence of an in-plane anisotropy of the magnetic susceptibility below T_h, which breaks the four-fold rotational symmetry of the tetragonal URu2Si2. Two-fold oscillations in the magnetic torque under in-plane field rotation were sensitively detected in small pure crystals. Our findings suggest that the h…
We report a layered ternary selenide BaPt4Se6 featuring sesqui-selenide Pt2Se3 layers sandwiched by Ba atoms. The Pt2Se3 layers in this compound can be derived from the Dirac-semimetal PtSe2 phase with Se vacancies that form a honeycomb structure. This structure results in a Pt (VI) and Pt (II) mixed-valence compound with both PtSe6 octahedra and PtSe4 square net coordination configurations. Temperature dependent electrical transport measurements suggest two distinct anomalies: a resistivity crossover, mimic to the metal-insulator (M-I) transition at ~150K, and a resistivity plateau at tempera…
One of the biggest puzzles concerning the cuprate high temperature superconductors is what determines the maximum transition temperature (Tc,max), which varies from less than 30 K to above 130 K in different compounds. Despite this dramatic variation, a robust trend is that within each family, the double-layer compound always has higher Tc,max than the single-layer counterpart. Here we use scanning tunneling microscopy to investigate the electronic structure of four cuprate parent compounds belonging to two different families. We find that within each family, the double layer compound has a mu…
Ultrathin sheets of transition metal dichalcogenides (MX$ _2$) with charge density waves (CDWs) is increasingly gaining interest as a promising candidate for graphene-like devices. Although experimental data including stripe/quasi-stripe structure and hidden states have been reported, the ground state of ultrathin MX$ _2$ compounds and, in particular, the origin of anisotropic (stripe and quasi-stripe) CDW phases is a long-standing problem. Anisotropic CDW phases have been explained by Coulomb interaction between domain walls and inter-layer interaction. However, these models assume that aniso…
To elucidate the underlying nature of the hidden order (HO) state in heavy-fermion compound URu2Si2, we measure electrical transport properties of ultraclean crystals in a high field/low temperature regime. Unlike previous studies, the present system with much less impurity scattering resolves a distinct anomaly of the Hall resistivity at H*=22.5 T well below the destruction field of the HO phase ~36 T. In addition, a novel quantum oscillation appears above a magnetic field slightly below H*. These results indicate an abrupt reconstruction of the Fermi surface, which implies a possible phase t…
An attractive proposal for the hidden order (HO) in the heavy electron compound URu2Si2 is an itinerant multipole order of high rank. It is due to the pairing of electrons and holes centered on zone center and boundary, respectively in states that have maximally different total angular momentum components. Due to the pairing with commensurate zone boundary ordering vector the translational symmetry is broken and a HO quasiparticle gap opens below the transition temperature T_HO. Inelastic neutron scattering (INS) has demonstrated that for T<T_HO the collective magnetic response is dominated by…
In low-dimensional metallic systems, lattice distortion is usually coupled to a density-wave-like electronic instability due to Fermi surface nesting (FSN) and strong electron-phonon coupling. However, the ordering of other electronic degrees of freedom can also occur simultaneously with the lattice distortion thus challenges the aforementioned prevailing scenario. Recently, a hidden electronic reconstruction beyond FSN was revealed in a layered metallic compound BaTi2As2O below the structural transition temperature Ts ~ 200 K. The nature of this hidden electronic instability is under strong d…
