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The pyrochlore metal Cd2Re2O7 has been recently investigated by second-harmonic generation (SHG) reflectivity. In this paper, we develop a general formalism that allows for the identification of the relevant tensor components of the SHG from azimuthal scans. We demonstrate that the secondary order parameter identified by SHG at the structural phase transition is the x2-y2 component of the axial toroidal quadrupole. This differs from the 3z2-r2 symmetry of the atomic displacements associated with the I-4m2 crystal structure that was previously thought to be its origin. Within the same formalism, we suggest that the primary order parameter detected in the SHG experiment is the 3z2-r2 component of the magnetic quadrupole. We discuss the general mechanism driving the phase transition in our proposed framework, and suggest experiments, particularly resonant X-ray scattering ones, that could clarify this issue.
Second harmonic generation (SHG) on the pyrochlore metal Cd2Re2O7 indicates the presence of three order parameters setting in below an inversion breaking transition. Here, we explore a possible structural explanation and relate it not only to the SHG data, but also to neutron and x-ray diffraction, where we find that such a structural scenario can explain certain reflection extinctions observed in single crystal x-ray data. From this analysis, we suggest future experiments that could be done to resolve this matter. Finally, we comment on the Landau-violating nature of the inversion breaking transition and its relation to similar phenomena observed in improper ferroelectrics.
The frustrated pyrochlore antiferromagnet Gd$_{2}$Ti$_{2}$O$_{7}$ has an unusual partially-ordered magnetic structure at the lowest measurable temperatures. This structure is currently believed to involve four magnetic propagation vectors $mathbf{k}in langle frac{1}{2} frac{1}{2} frac{1}{2} rangle^*$ in a cubic 4-$mathbf{k}$ structure, based on analysis of magnetic diffuse-scattering data [J. Phys.: Condens. Matter 16, L321 (2004)]. Here, we present three pieces of evidence against the 4-$mathbf{k}$ structure. First, we report single-crystal neutron-diffraction measurements as a function of applied magnetic field, which are consistent with the selective field-induced population of non-cubic magnetic domains. Second, we present evidence from high-resolution powder neutron-diffraction measurements that rhombohedral strains exist within magnetic domains, which may be generated by magneto-elastic coupling only for the alternative 1-$mathbf{k}$ structure. Finally, we show that the argument previously used to rule out the 1-$mathbf{k}$ structure is flawed, and demonstrate that magnetic diffuse-scattering data can actually be fitted quantitatively by a 1-$mathbf{k}$ structure in which spin fluctuations on ordered and disordered magnetic sites are strongly coupled. Our results provide an experimental foundation on which to base theoretical descriptions of partially-ordered states.
Partially-ordered magnets are distinct from both spin liquids and conventional ordered magnets because order and disorder coexist in the same magnetic phase. Here, we determine the nature of partial order in the canonical frustrated pyrochlore antiferromagnet Gd$_2$Ti$_{2}$O$_{7}$. Using single-crystal neutron-diffraction measurements in applied magnetic field, magnetic symmetry analysis, inelastic neutron-scattering measurements, and spin-wave modeling, we show that its low-temperature magnetic structure involves two propagation vectors (2-$mathbf{k}$ structure) with suppressed ordered magnetic moments and enhanced spin-wave fluctuations. Our experimental results support theoretical predictions of thermal fluctuation-driven order in Gd$_{2}$Ti$_{2}$O$_{7}$.
Superconductors with kagome lattices have been identified for over 40 years, with a superconducting transition temperature TC up to 7K. Recently, certain kagome superconductors have been found to exhibit an exotic charge order, which intertwines with superconductivity and persists to a temperature being one order of magnitude higher than TC. In this work, we use scanning tunneling microscopy (STM) to study the charge order in kagome superconductor RbV3Sb5. We observe both a 2x2 chiral charge order and nematic surface superlattices (predominantly 1x4). We find that the 2x2 charge order exhibits intrinsic chirality with magnetic field tunability. Defects can scatter electrons to introduce standing waves, which couple with the charge order to cause extrinsic effects. While the chiral charge order resembles that discovered in KV3Sb5, it further interacts with the nematic surface superlattices that are absent in KV3Sb5 but exist in CsV3Sb5.
Kagome superconductors with Tc up to 7K have been discovered over 40 years. Recently, unconventional chiral charge order has been reported in kagome superconductor KV3Sb5, with an ordering temperature of one order of magnitude higher than the TC. However, the chirality of the charge order has not been reported in the cousin kagome superconductor CsV3Sb5, and the electronic nature of the chirality remains elusive. In this letter, we report the observation of electronic chiral charge order in CsV3Sb5 via scanning tunneling microscopy (STM). We observe a 2x2 charge modulation and a 1x4 superlattice in both topographic data and tunneling spectroscopy. 2x2 charge modulation is highly anticipated as a charge order by fundamental kagome lattice models at van Hove filling, and is shown to exhibit intrinsic chirality. We find that the 1x4 superlattices forms various small domain walls, and can be a surface effect as supported by our first-principles calculations. Crucially, we find that the amplitude of the energy gap opened by the charge order exhibits real space modulations, and features 2x2 wave vectors with chirality, highlighting the electronic nature of the chiral charge order. STM study at 0.4K reveals a superconducting energy gap with a gap size 2{Delta}=0.85meV, which estimates a moderate superconductivity coupling strength with 2{Delta}/kBTc=3.9. When further applying a c-axis magnetic field, vortex core bound states are observed within this gap, indicative of clean-limit superconductivity.