Evidence of symmetry lowering in antiferromagnetic metal TmB12with dynamic charge stripes.

Precise angle-resolved magnetoresistance (ARMR) and magnetization measurements have revealed (i) strong charge transport and magnetic anisotropy and (ii) emergence of a huge number of magnetic phases in the ground state of isotopically11B-enriched single crystals of TmB12antiferromagnetic (AF) metal with fcc crystal structure and dynamic charge stripes. We analyze for the first time the angularH-φphase diagrams of AF state of Tm11B12reconstructed from experimental ARMR and magnetization data arguing that the symmetry lowering leads to the appearance of several radial phase boundaries between different phases in the AF state. It is proposed that the suppression of the indirect Ruderman-Kittel-Kasuya-Yosida (RKKY) exchange along ⟨110⟩ directions between nearest neighboring magnetic moments of Tm3+ions and subsequent redistribution of conduction electrons to quantum fluctuations of the electron density (dynamic stripes) are the main factors responsible for the anisotropy. Essential (more than 25% atT= 2 K) anisotropy of the Neel field in the (110) plane was found in Tm11B12unlike to isotropic AF-P boundary in theH-φphase diagrams of Ho11B12. Magnetoresistance components are discussed in terms of charge carrier scattering on the spin density wave, itinerant ferromagnetic nano-domains and on-site Tm3+spin fluctuations.

Role of spin-glass behavior in the formation of exotic magnetic states in GdB6.

Randomness and frustration are believed to be two crucial criteria for the formation of spin glass state. However, the spin freezing occurs in some well-ordered crystals below the related temperature Tf due to the instability of each spin state, which induces the variation of either magnetic moment value or exchange energy. Here we explore the new mechanism of the in-site originated disorder in antiferromagnets Gd0.73La0.27B6 and GdB6, which is caused by the random mutual shifts of Gd3+ spins from the centrally symmetrical positions in the regular cubic lattice. The universal scaling of ESR linewidth temperature dependencies to the power law ΔH(T) ~ ((T - TD)/TD)α with α = - 1.1 ± 0.05 in the paramagnetic phase of both compounds demonstrates the identity of the origin of magnetic randomness. In Gd0.73La0.27B6 the resulting random spin configurations freeze at Tf ≈ 10.5 K where the maximum of magnetization is observed. Below Tf the splitting of ZFC and FC magnetization curves takes place as well as the magnetic state depends on the antecedent sample history. In the case of GdB6 the coherent displacement of Gd ions compete with these random shifts forming an antiferromagnetic (AFM) phase at TN = 15.5 K, which prevails over the spin freezing at Tf ≈ 13 K, expected from the ESR data. The observation of the hysteresis of the ESR spectrum in the AFM phase suggests that its properties may be determined by the competition of two types of AFM orders, which results in formation of stable magnetic domains with nonequivalent positions of AFM Gd pairs at T < 10 K.

Evolution of thermoelectric properties in EuxYb1-xB6 family.

Seebeck effect in the crystalline samples of EuxYb1-xB6 (x = 0, 0.082, 0.127, 0.9, 1) was investigated at temperatures 2-300 K. For all the compounds thermopower is shown to be well described by the sum of diffusion (S d = AT) and phonon drag components. The latter contribution is induced by quasilocal (Einstein) modes of ytterbium and europium ions with characteristic temperatures ΘE(YbB6) ≈ 91 K and ΘE(EuB6) ≈ 122 K. The estimation of effective mass m * of the charge carriers proves that increasing of Eu content induces crossover from 'heavy' holes with m h *(x ⩽ 0.127) ≈ 0.3-0.36 m 0 to 'light' electrons with m e *(x ⩾ 0.9) ≈ 0.12-0.13 m 0 (m 0-free electron mass). For the Eu-rich compounds we propose the existence of additional point on the phase diagram, which corresponds to short-range magnetic order with enhanced spin fluctuations preceding the stabilization of magnetic polarons.

Observation of dynamic charge stripes in Tm0.19Yb0.81B12 at the metal-insulator transition.

Accurate low temperature charge transport measurements in combination with high-precision x-ray diffraction experiments have allowed detection of the symmetry lowering in the single domain Tm0.19Yb0.81B12 crystals that belong to the family of dodecaborides with metal-insulator transition. Based on the fine structure analysis we discover the formation of dynamic charge stripes within the semiconducting matrix of Tm0.19Yb0.81B12. The charge dynamics in these conducting nano-size channels is characterized by broad-band optical spectroscopy that allowed estimating the frequency (~2.4 × 1011 Hz) of quantum motion of the charge carriers. It is suggested that cooperative Jahn-Teller effect in the boron sublattice is a cause of the large-amplitude rattling modes of the Tm and Yb ions responsible for the 'modulation' of the conduction band along one of the [Formula: see text] directions through the variation of 5d-2p hybridization of electron states.

Magnetic resonance probing of ground state in the mixed valence correlated topological insulator SmB6.

Introducing of topological insulator concept for fluctuating valence compound - samarium hexaboride - has recently initiated a new round of studies aimed to clarify the nature of the ground state in this extraordinary system with strong electron correlations. Here we discuss the data of magnetic resonance in the pristine single crystals of SmB6 measured in 60 GHz cavity experiments at temperatures 1.8-300 K. The microwave study as well as the DC resistivity and Hall effect measurements performed for the different states of SmB6 [110] surface prove definitely the existence of the layer with metallic conductivity increasing under lowering temperature below 5 K. Four lines with the g-factors g ≈ 2 are found to contribute to the ESR-like absorption spectrum that may be attributed to intrinsic paramagnetic centers on the sample's surface, which are robust with respect to the surface treatment. The temperature dependence of integrated intensity I(T) for main paramagnetic signal is found to demonstrate anomalous critical behavior I(T) ~ (T* - T)ν with characteristic temperature T * = 5.34 ± 0.05 K and exponent ν = 0.38 ± 0.03 indicating possible magnetic transition at the SmB6 [110] surface. Additional resonant magnetoabsorption line, which may be associated with either donor-like defects or cyclotron resonance mode corresponding to the mass m c ~ 1.2m0, is reported.

Samarium hexaboride is a trivial surface conductor.

SmB6 is predicted to be the first member of the intersection of topological insulators and Kondo insulators, strongly correlated materials in which the Fermi level lies in the gap of a many-body resonance that forms by hybridization between localized and itinerant states. While robust, surface-only conductivity at low temperature and the observation of surface states at the expected high symmetry points appear to confirm this prediction, we find both surface states at the (100) surface to be topologically trivial. We find the [Formula: see text] state to appear Rashba split and explain the prominent [Formula: see text] state by a surface shift of the many-body resonance. We propose that the latter mechanism, which applies to several crystal terminations, can explain the unusual surface conductivity. While additional, as yet unobserved topological surface states cannot be excluded, our results show that a firm connection between the two material classes is still outstanding.

Electron nematic effect induced by magnetic field in antiferroquadrupole phase of CeB 6.

Spatial anisotropy generated spontaneously in the translationally invariant metallic phase, i.e. electron nematic effect, addresses a great challenge for both experimentalists and theoreticians. An interesting option for the realization of the electron nematic phase is provided by the system with orbital ordering, as long as both orbitally ordered states and electron nematic phases possess broken spatial symmetry. Here we report the detailed study of the angular dependences of the magnetoresistance in the orbitally ordered antiferroquadrupole (AFQ) phase of CeB6. Our data allowed revealing the electron nematic effect, which develops when magnetic field exceeds a critical value of 0.3-0.5T. As a result, new transition inside the AFQ phase corresponding to the change of the symmetry of magnetic scattering on spin fluctuations in CeB6 is discovered.

Magnetic resonance anisotropy in CeB6: an entangled state of the art.

Electron spin resonance (ESR) in strongly correlated metals is an exciting phenomenon, as strong spin fluctuations in this class of materials broaden extremely the absorption line below the detection limit. In this respect, ESR observation in CeB6 provides a unique chance to inspect Ce3+ magnetic state in the antiferroquadrupole (AFQ) phase. We apply the original high frequency (60 GHz) experimental technique to extract the temperature and angular dependences of g-factor, line width and oscillating magnetization. Experimental data show unambiguously that the modern ESR theory in the AFQ phase considering the Γ8 ground state of Ce3+ ion completely fails to predict both the g-factor magnitude and its angular dependence. Alignment of the external magnetic field along [100] axis induces a strong (more than twofold) broadening of ESR line width with respect to the other crystallographic directions and results also in the anomalous temperature dependences of the g-factor and oscillating magnetization. In this experimental geometry the latter parameter surprisingly exceeds total static magnetization by 20% at T* ~ 2.5 K. We argue that the unusual physical picture of ESR in CeB6 may be strongly affected by spin fluctuations and dynamic collective effects predominantly pronounced in [100] direction.

Nesting-driven multipolar order in CeB6 from photoemission tomography.

Some heavy fermion materials show so-called hidden-order phases which are invisible to many characterization techniques and whose microscopic origin remained controversial for decades. Among such hidden-order compounds, CeB6 is of model character due to its simple electronic configuration and crystal structure. Apart from more conventional antiferromagnetism, it shows an elusive phase at low temperatures, which is commonly associated with multipolar order. Here we show that this phase roots in a Fermi surface instability. This conclusion is based on a full 3D tomographic sampling of the electronic structure by angle-resolved photoemission and comparison with inelastic neutron scattering data. The hidden order is mediated by itinerant electrons. Our measurements will serve as a paradigm for the investigation of hidden-order phases in f-electron systems, but also generally for situations where the itinerant electrons drive orbital or spin order.

Intense low-energy ferromagnetic fluctuations in the antiferromagnetic heavy-fermion metal CeB6.

Heavy-fermion metals exhibit a plethora of low-temperature ordering phenomena . Among these are the so-called hidden-order phases that, in contrast to conventional magnetic order, are invisible to standard neutron diffraction experiments. One of the structurally most simple hidden-order compounds, CeB6, has been intensively studied for an elusive phase that was attributed to the antiferroquadrupolar ordering of cerium-4f moments . As the ground state of CeB6 is characterized by a more conventional antiferromagnetic (AFM) order , the low-temperature physics of this system has generally been assumed to be governed solely by AFM interactions between the dipolar and multipolar Ce moments . Here we overturn this established picture by observing an intense ferromagnetic (FM) low-energy collective mode that dominates the magnetic excitation spectrum of CeB6. Inelastic neutron-scattering data reveal that the intensity of this FM excitation significantly exceeds that of conventional spin-wave magnons emanating from the AFM wavevectors, thus placing CeB6 much closer to a FM instability than previously anticipated. This propensity for ferromagnetism may account for much of the unexplained behaviour of CeB6, and should lead to a re-examination of existing theories that have so far largely neglected the role of FM interactions.

Isotopic phonon effects in LaB6-LaB6 do not possess cubic symmetry and show a non-random isotope distribution.

The isotopic phonon effects in LaB(6) are investigated on the Raman spectra of a series of high-quality single crystals with systematically varied contents of (10)B and (11)B isotopes. A detailed group theoretical analysis enlightens the correlation between distortions of the B(6) octahedra and the splitting or broadening of phonon modes. It is evident that LaB(6) does not have cubic symmetry as assumed so far. A further symmetry reduction of the B(6) octahedra occurs in isotopically mixed crystals. There, the distribution of isotopes is not random as commonly assumed; the probability of associating equal isotopes increases with their mass decreasing.

Resonant magnetic exciton mode in the heavy-fermion antiferromagnet CeB6.

Resonant magnetic excitations are recognised as hallmarks of unconventional superconductivity in copper oxides, iron pnictides and heavy-fermion compounds. Model calculations have related these modes to the microscopic properties of the pair wave function, but the mechanisms of their formation are still debated. Here we report the discovery of a similar resonant mode in the non-superconducting antiferromagnetic heavy-fermion metal CeB(6). Unlike conventional magnons, the mode is non-dispersive and is sharply peaked around a wave vector separate from those characterising the antiferromagnetic order. It is likely associated with a co-existing order parameter of the unusual antiferro-quadrupolar phase of CeB(6), which has long remained hidden to neutron-scattering probes. The mode energy increases continuously below the onset temperature for antiferromagnetism, in parallel to the opening of a nearly isotropic spin gap throughout the Brillouin zone. These attributes are similar to those of the resonant modes in unconventional superconductors. This unexpected commonality between the two disparate ground states indicates the dominance of itinerant spin dynamics in the ordered low-temperature phases of CeB(6) and throws new light on the interplay between antiferromagnetism, superconductivity and 'hidden' order parameters in correlated-electron materials.

Raman scattering and isotopic phonon effects in dodecaborides.

The Raman spectra of numerous dodecaborides have been measured on high-quality single crystals at ambient conditions with high spectral resolution and signal-to-noise ratio. Besides the strong Raman-active modes, numerous Raman-inactive modes occur in the spectra, indicating distortions of the structures. Ab initio calculation of the phonon spectra on ZrB(12) excellently agrees with the experimental results. Force constants are theoretically calculated and force parameters are estimated from the Raman frequencies. The influence of the surface range on the Raman spectra is evident. The different isotopic effects (virtual crystal approximation, the polarization effect and the effect of isotopic disorder) on the phonon frequencies are determined, separated and discussed.

Surface superconducting states in a yttrium hexaboride single crystal in a tilted magnetic field.

We present the results of an experimental study of the nucleation of superconductivity at the surface of a single-crystal YB(6) in a tilted dc magnetic field. The developed experimental approach allowed us to measure H(c3) at each side of the sample as a function of the angle between the dc magnetic field and the surface. Experiment showed that the ratio H(c3)/H(c2)≈1.28 when the dc field became perpendicular to the surface while the expected value of this ratio is 1. This sharp distinction with theory cannot be ascribed to the surface roughness.

Fractional magnetization plateaus and magnetic order in the Shastry-Sutherland magnet TmB4.

We investigate the phase diagram of TmB4, an Ising magnet on a frustrated Shastry-Sutherland lattice, by neutron diffraction and magnetization experiments. At low temperature we find Néel order at low field, ferrimagnetic order at high field, and an intermediate phase with magnetization plateaus at fractional values M/M_(sat)=1/7,1/8,1/9,... and spatial stripe structures. Using an effective S=1/2 model and its equivalent two-dimensional fermion gas we suggest that the magnetic properties of TmB4 are related to the fractional quantum Hall effect of a 2D electron gas.

Effect of pressure on the Ginzburg-Landau parameter kappa=lambda/xi in YB6.

Measurements of the transition temperature Tc, the upper critical field Hc2, and the magnetic penetration depth lambda under hydrostatic pressure (up to approximately 9.2 kbar) in the YB6 superconductor were carried out. A pronounced and negative pressure effect (PE) on Tc and Hc2 with dTc/dp=-0.0547(4) K/kbar and micro0dHc2(0)/dp=-4.84(20) mT/kbar, and zero PE on lambda(0) were observed. The PE on the coherence length dxi(0)/dp=0.28(2) nm/kbar was calculated from the measured pressure dependence of Hc2(0). Together with the zero PE on the magnetic penetration depth lambda(0), our results imply that the Ginzburg-Landau parameter kappa(0)=xi(0)/lambda(0) depends on pressure and that pressure "softens" YB6, e.g., moves it to the type-I direction.