We investigated the electronic structure of the enigmatic CeRh_3B_2 using resonant inelastic scattering and x-ray absorption spectroscopy in combination with ab initio density functional calculations. We find that the Rh 4d states are irrelevant for the high-temperature ferromagnetism and the Kondo effect. We also find that the Ce 4f crystal-field strength is too small to explain the strong reduction of the Ce magnetic moment. The data reveal instead the presence of two different active Ce 4f orbitals, with each coupling selectively to different bands in CeRh_3B_2. The inter-site hybridization of the |J=5/2,Jz=+/-1/2> crystal-field state and Ce 5d band combined with the intra-site Ce 4f-5d exchange creates the strong ferromagnetism, while hybridization between the |J=5/2,Jz=+/-5/2> and the B sp in the ab-plane contributes to the Kondo interaction which causes the moment reduction. This orbital selective coupling explains the unique and seemingly contradictory properties of CeRh_3B_2.
By combining inelastic neutron scattering and numerical simulations, we study the quasi-one-dimensional Ising-like quantum antiferromagnet BaCo2V2O8 in a longitudinal magnetic field applied along the Ising anisotropy, which is also the chain direction. The external field closes the excitation gap due to the magnetic anisotropy, inducing a transition from the Neel ordered state to an incommensurate longitudinal spin density wave phase. If the field is increased further, another transition into a transverse antiferromagnetic phase takes place at 9 T due to the competition between longitudinal and transverse correlations. We numerically and experimentally show that the model of XXZ chains connected by a weak interchain interaction well reproduces this transition. We also calculate the dynamical susceptibility and demonstrate that it agrees quantitatively with inelastic neutron scattering measurements. In contrast to the abrupt change of magnetic ordering, the spectra do not change much at the transition at 9 T, and the spin dynamics can be described as a Tomonaga-Luttinger liquid. We also refine the modeling of BaCo2V2O8 by including a four-site periodic term arising from the crystal structure which enables one to account for an anomaly of the magnetic susceptibility appearing at 19.5 T, as well as for the anticrossing observed in the inelastic neutron scattering spectra.
Geometrical frustration, as in pyrochlore lattices made of corner-sharing tetrahedra, precludes the onset of conventional magnetic ordering, enabling the stabilization of fluctuating spin states at low temperature. Disorder is a subtle ingredient that can modify the nature of these exotic non-ordered phases. Here, we study the interplay between disorder and magnetic frustration in the new pyrochlore Tb$_{2}$ScNbO$_{7}$ where the non magnetic site presents a charge disorder Nb$^{5+}$/Sc$^{3+}$. Its quantification with sophisticated diffraction techniques (electrons, X-rays, neutrons) allows us to estimate the distribution of the splitting of the magnetic Tb$^{3+}$ non-Kramers ground state doublets and to compare it with excitations measured in inelastic neutron scattering. Combining macroscopic and neutron scattering measurements, we show that a clear spin glass transition at 1 K stems out while retaining strong spin liquid correlations. Our results suggest that Tb$_{2}$ScNbO$_{7}$ stabilizes one of the novel disorder induced quantum spin liquid or topological glassy phases recently proposed theoretically.
In matter, any spontaneous symmetry breaking induces a phase transition characterized by an order parameter, such as the magnetization vector in ferromagnets, or a macroscopic many electron wave function in superconductors. Phase transitions with unknown order parameter are rare but extremely appealing, as they may lead to novel physics. An emblematic and still unsolved example is the transition of the heavy fermion compound URu2Si2 (URS) into the so-called hidden-order (HO) phase when the temperature drops below T-0 = 17.5 K. Here, we show that the interaction between the heavy fermion and the conduction band states near the Fermi level has a key role in the emergence of the HO phase. Using angle-resolved photoemission spectroscopy, we find that while the Fermi surfaces of the HO and of a neighboring antiferromagnetic (AFM) phase of well-defined order parameter have the same topography, they differ in the size of some, but not all, of their electron pockets. Such a nonrigid change of the electronic structure indicates that a change in the interaction strength between states near the Fermi level is a crucial ingredient for the HO to AFM phase transition.
We study the dynamics of the quasi-one-dimensional Ising-Heisenberg antiferromagnet BaCo2V2O8 under a transverse magnetic field. Combining inelastic neutron scattering experiments and theoretical analyses by field theories and numerical simulations, we mainly elucidate the structure of the spin excitation spectrum in the high field phase, appearing above the quantum phase transition point mu0Hc 10 T. We find that it is characterized by collective solitonic excitations superimposed on a continuum. These solitons are strongly bound in pairs due to the effective staggered field induced by the nondiagonal g tensor of the compound, and are topologically different from the fractionalized spinons in the weak field region. The dynamical susceptibility numerically calculated with the infinite time-evolving block decimation method shows an excellent agreement with the measured spectra, which enables us to identify the dispersion branches with elementary excitations. The lowest energy dispersion has an incommensurate nature and has a local minimum at an irrational wave number due to the applied transverse field.
We report on a comprehensive investigation of the effects of strain and film thickness on the structural and magnetic properties of epitaxial thin films of the prototypal $J_\mathrm{eff}=1/2$ compound Sr$_2$IrO$_4$ by advanced X-ray scattering. We find that the Sr$_2$IrO$_4$ thin films can be grown fully strained up to a thickness of 108 nm. By using X-ray resonant scattering, we show that the out-of-plane magnetic correlation length is strongly dependent on the thin film thickness, but independent of the strain state of the thin films. This can be used as a finely tuned dial to adjust the out-of-plane magnetic correlation length and transform the magnetic anisotropy from two-dimensional (2D) to three-dimensional (3D) behavior by incrementing film thickness. These results provide a clearer picture for the systematic control of the magnetic degrees of freedom in epitaxial thin films of Sr$_2$IrO$_4$ and bring to light the potential for a rich playground to explore the physics of $5d$-transition metal compounds.
We report on a comprehensive investigation of the effects of strain and film thickness on the structural and magnetic properties of epitaxial thin films of the prototypal J(eff) = 1/2 compound Sr2IrO4 by advanced x-ray scattering. We find that the Sr2IrO4 thin films can be grown fully strained up to a thickness of 108 nm. By using x-ray resonant scattering, we show that the out-of-plane magnetic correlation length is strongly dependent on the thin film thickness, but independent of the strain state of the thin films. This can be used as a finely tuned dial to adjust the out-of-plane magnetic correlation length and transform the magnetic anisotropy from two-dimensional to three-dimensional behavior by incrementing film thickness. These results provide a clearer picture for the systematic control of the magnetic degrees of freedom in epitaxial thin films of Sr2IrO4 and bring to light the potential for a rich playground to explore the physics of 5d transition-metal compounds.
We report a ground state with strongly coupled magnetic and charge density wave orders mediated via orbital ordering in the layered compound \tbt. In addition to the commensurate antiferromagnetic (AFM) and charge density wave (CDW) orders, new magnetic peaks are observed whose propagation vector equals the sum of the AFM and CDW propagation vectors, revealing an intricate and highly entwined relationship. This is especially interesting given that the magnetic and charge orders lie in different layers of the crystal structure where the highly localized magnetic moments of the Tb$^{3+}$ ions are netted in the Tb-Te stacks, while the charge order is formed by the conduction electrons of the adjacent Te-Te layers. Our results, based on neutron diffraction and resonant x-ray scattering reveal that the charge and magnetic subsystems mutually influence each other via the orbital ordering of Tb$^{3+}$ ions.
Anisotropic multiferroic properties of SrMnGe2O6 pyroxene single crystals were systematically investigated by means of magnetization, heat capacity, pyroelectric current measurement and elastic and inelastic neutron scattering experiments. Single crystal neutron diffraction allows us to unambiguously reveal the presence of two incommensurate magnetic orderings: a non-polar amplitude-modulated collinear sinusoidal magnetic structure emerges at TN1=4.36(2)K followed by a polar elliptical cycloidal spin structure below TN2=4.05(2)K. Pyroelectric current measurements on single crystal confirm the appearance of a spontaneous polarization within the (ac) plane below TN2 associated with the latter magnetic symmetry through extended Dzyaloshinsky-Moriya mechanism. The magnetic phase diagram was calculated considering the three isotropic exchange couplings relevant in this system. The magnetic excitations spectra of SrMnGe2O6 measured by inelastic neutron scattering were successfully modeled using a set of exchange interactions consistent with this phase diagram.
Co2+ ions in an octahedral crystal field stabilize a j(eff) = 1/2 ground state with an orbital degree of freedom and have been recently put forward for realizing Kitaev interactions, a prediction we have tested by investigating spin dynamics in two cobalt honeycomb lattice compounds, Na2Co2TeO6 and Na3Co2SbO6, using inelastic neutron scattering. We used linear spin wave theory to show that the magnetic spectra can be reproduced with a spin Hamiltonian including a dominant Kitaev nearest-neighbor interaction, weaker Heisenberg interactions up to the third neighbor, and bond-dependent off-diagonal exchange interactions. Beyond the Kitaev interaction that alone would induce a quantum spin liquid state, the presence of these additional couplings is responsible for the zigzag-type long-range magnetic ordering observed at low temperature in both compounds. These results provide evidence for the realization of Kitaev-type coupling in cobalt-based materials, despite hosting a weaker spin-orbit coupling than their 4d and 5d counterparts.
We report on a comprehensive investigation of the effects of strain and film thickness on the structural and magnetic properties of epitaxial thin films of the prototypal $J_\mathrm{eff}=1/2$ compound Sr$_2$IrO$_4$ by advanced X-ray scattering. We find that the Sr$_2$IrO$_4$ thin films can be grown fully strained up to a thickness of 108 nm. By using X-ray resonant scattering, we show that the out-of-plane magnetic correlation length is strongly dependent on the thin film thickness, but independent of the strain state of the thin films. This can be used as a finely tuned dial to adjust the out-of-plane magnetic correlation length and transform the magnetic anisotropy from two-dimensional (2D) to three-dimensional (3D) behavior by incrementing film thickness. These results provide a clearer picture for the systematic control of the magnetic degrees of freedom in epitaxial thin films of Sr$_2$IrO$_4$ and bring to light the potential for a rich playground to explore the physics of $5d$-transition metal compounds.
Neutron scattering, specific heat and magnetisation measurements on both powders and single crystals reveal that Dy$_2$Ir$_2$O$_7$ realizes the fragmented monopole crystal state in which antiferromagnetic order and a Coulomb phase spin liquid co-inhabit. The measured residual entropy is that of a hard core dimer liquid, as predicted. Inclusion of Coulomb interactions allows for a quantitative description of both the thermodynamic data and the magnetisation dynamics, with the energy scale given by deconfined defects in the emergent ionic crystal. Our data reveal low energy excitations, as well as a large distribution of energy barriers down to low temperatures, while the magnetic response to an applied field suggests that domain wall pinning is important; results that call for further theoretical modelling.
The influence of a staggered molecular field in frustrated rare-earth pyrochlores, produced via the magnetic iridium occupying the transition metal site, can generate exotic ground states, such as the fragmentation of the magnetization in the Ho compound. At variance with the Ising Ho$^{3+}$ moment, we focus on the behavior of the quasi isotropic magnetic moment of the Gd$^{3+}$ ion at the rare-earth site. By means of macroscopic measurements and neutron scattering, we find a complex situation where different components of the magnetic moment contribute to two antiferromagnetic non-collinear arrangements: a high temperature all in - all out order induced by the Ir molecular field, and Palmer and Chalker correlations that tend to order at much lower temperatures. This is enabled by the anisotropic nature of the Gd-Gd interactions and requires a weak easy-plane anisotropy of the Gd$^{3+}$ moment due to the mixing of the ground state with multiplets of higher spectral terms.
Magnetic ground states with peculiar spin textures, such as magnetic skyrmions and multifunctional domains are of enormous interest for the fundamental physics governing their origin as well as potential applications in emerging technologies. Of particular interest are multiferroics, where sophisticated interactions between electric and magnetic phenomena can be used to tailor several functionalities. We report the direct observation of a magnetic field induced long-wavelength spin spiral modulation in the chiral compound Ba _3 TaFe _3 Si _2 O _14 , which emerges out of a helical ground state, and is hallmarked by the onset of a unique chirality-dependent contribution to the bulk electric polarization. The periodicity of the field-induced modulation, several hundreds of nm depending on the field value, is comparable to the length scales of mesoscopic topological defects such as skyrmions, merons, and solitons. The phase transition and observed threshold behavior are consistent with a phenomenology based on the allowed Lifshitz invariants for the chiral symmetry of langasite, which intriguingly contain all the essential ingredients for the realization of topologically stable antiferromagnetic skyrmions. Our findings open up new directions to explore topological correlations of antiferromagnetic spintronic systems based on non-collinear magnetic systems with additional ferroic functionalities.
Combining inelastic neutron scattering and numerical simulations, we study the quasi-one-dimensional Ising anisotropic quantum antiferromagnet BaCo_{2}V_{2}O_{8} in a longitudinal magnetic field. This material shows a quantum phase transition from a Néel ordered phase at zero field to a longitudinal incommensurate spin density wave at a critical magnetic field of 3.8 T. Concomitantly, the excitation gap almost closes and a fundamental reconfiguration of the spin dynamics occurs. These experimental results are well described by the universal Tomonaga-Luttinger liquid theory developed for interacting spinless fermions in one dimension. We especially observe the rise of mainly longitudinal excitations, a hallmark of the unconventional low-field regime in Ising-like quantum antiferromagnetic chains.
Our measurements of the Hall coefficient in rare-earth tritelluride compounds reveal a strong hysteresis between cooling and warming in the low temperature range where a second unidirectional charge density wave (CDW) occurs. We show that this effect results from the interplay between two instabilities: band crossing of the Te $p_{x}$ and $p_{y}$ orbitals at the Fermi level and CDW, which have a close energy gain and compete. Calculation of the electron susceptibility at the CDW wave vector with and without band anticrossing reconstruction of the electron spectrum yields a satisfactory estimation of the temperature range of the hysteresis in Hall effect measurements.
Since the seminal ideas of Berezinskii, Kosterlitz and Thouless, topological excitations have been at the heart of our understanding of a whole novel class of phase transitions. In most cases, those transitions are controlled by a single type of topological objects. There are, however, some situations, still poorly understood, where two dual topological excitations fight to control the phase diagram and the transition. Finding experimental realizations of such cases is thus of considerable interest. We show here that this situation occurs in BaCo 2 V 2 O 8 , a spin-1/2 Ising-like quasi-one-dimensional antiferromagnet, when subjected to a uniform magnetic field transverse to the Ising axis. Using neutron scattering experiments, we measure a drastic modification of the quantum excitations beyond a critical value of the magnetic field. This quantum phase transition is identified, through a comparison with theoretical calculations, to be a transition between two different types of solitonic topological object, which are captured by different components of the dynamical structure factor.
We present ultrasonic measurements on the rare earth tritelluride HoTe3 compound. Different anomalies are observed at the upper and lower charge density wave phase transition T[Formula: see text] = 284 K and T[Formula: see text] = 120 K. A striking T2 temperature dependence of the velocities of the longitudinal C[Formula: see text], C[Formula: see text] and shear C[Formula: see text] modes is observed in the ordered phase below the lower CDW phase transition T[Formula: see text]. Such a behavior is related to the temperature dependence of the CDW order parameter.
In the version of this Letter originally published, the year for ref. 30 was incorrectly listed as 2009; it should have been 2004. This has now been corrected.