Search

Abstract Clarifying the underlying mechanisms that govern ordering transitions in condensed matter systems is crucial for comprehending emergent properties and phenomena. While transitions are often classified as electronically driven or lattice-driven, we present a departure from this conventional picture in the case of the double perovskite Ba2MgReO6. Leveraging resonant and non-resonant elastic x-ray scattering techniques, we unveil the simultaneous ordering of structural distortions and charge quadrupoles at a critical temperature of T q ~ 33 K. Using a variety of complementary first-principles-based computational techniques, we demonstrate that, while electronic interactions drive the ordering at T q, it is ultimately the lattice distortions that dictate the specific ground state that emerges. Our findings highlight the crucial interplay between electronic and lattice degrees of freedom, providing a unified framework to understand and predict unconventional emergent phenomena in quantum materials.

Abstract Exotic quantum phases, arising from a complex interplay of charge, spin, lattice and orbital degrees of freedom, are of immense interest to a wide research community. A well-known example of such an entangled behavior is the Jahn-Teller effect, where the lifting of orbital degeneracy proceeds through lattice distortions. Here we demonstrate that a highly-symmetrical 5d1 double perovskite Ba2MgReO6, comprising a 3D array of isolated ReO6 octahedra, represents a rare example of a dynamic Jahn-Teller system in the strong spin-orbit coupling regime. Thermodynamic and resonant inelastic x-ray scattering experiments, supported by quantum chemistry calculations, undoubtedly show that the Jahn-Teller instability leads to a ground-state doublet, resolving a long-standing puzzle in this family of compounds. The dynamic state of ReO6 octahedra persists down to the lowest temperatures, where a multipolar order sets in, allowing for investigations of the interplay between a dynamic JT effect and strongly correlated electron behavior.

Abstract Quantum spin liquids (QSLs) have become a key area of research in magnetism due to their remarkable properties, such as long-range entanglement, fractional excitations, and topologically protected phenomena. Recently, the search for QSLs has expanded into the three-dimensional world, despite the suppression of quantum fluctuations due to high dimensionality. A new candidate material, K2Ni2(SO4)3, belongs to the langbeinite family and consists of two interconnected trillium lattices. Although magnetically ordered, it exhibits a highly dynamical and correlated state. In this work, we combine inelastic neutron scattering measurements with density functional theory (DFT), pseudo-fermion functional renormalization group (PFFRG), and classical Monte Carlo (cMC) calculations to study the magnetic properties of K2Ni2(SO4)3, revealing a high level of agreement between experiment and theory. We further reveal the origin of the dynamical state in K2Ni2(SO4)3 to be centred around a magnetic network composed of tetrahedra on a trillium lattice.

Abstract In the rapidly expanding field of topological materials there is growing interest in systems whose topological electronic band features can be induced or controlled by magnetism. Magnetic Weyl semimetals, which contain linear band crossings near the Fermi level, are of particular interest owing to their exotic charge and spin transport properties. Up to now, the majority of magnetic Weyl semimetals have been realized in ferro- or ferrimagnetically ordered compounds, but a disadvantage of these materials for practical use is their stray magnetic field which limits the minimum size of devices. Here we show that Weyl nodes can be induced by a helical spin configuration, in which the magnetization is fully compensated. Using a combination of neutron diffraction and resonant elastic x-ray scattering, we find that below T N = 14.5 K the Eu spins in EuCuAs develop a planar helical structure which induces two quadratic Weyl nodes with Chern numbers C = ±2 at the A point in the Brillouin zone.

Abstract In quantum magnetic materials, ordered phases induced by an applied magnetic field can be described as the Bose-Einstein condensation (BEC) of magnon excitations. In the strongly frustrated system SrCu2(BO3)2, no clear magnon BEC could be observed, pointing to an alternative mechanism, but the high fields required to probe this physics have remained a barrier to detailed investigation. Here we exploit the first purpose-built high-field neutron scattering facility to measure the spin excitations of SrCu2(BO3)2 up to 25.9 T and use cylinder matrix-product-states (MPS) calculations to reproduce the experimental spectra with high accuracy. Multiple unconventional features point to a condensation of S = 2 bound states into a spin-nematic phase, including the gradients of the one-magnon branches and the persistence of a one-magnon spin gap. This gap reflects a direct analogy with superconductivity, suggesting that the spin-nematic phase in SrCu2(BO3)2 is best understood as a condensate of bosonic Cooper pairs.

Abstract Control of magnetization and electric polarization is attractive in relation to tailoring materials for data storage and devices such as sensors or antennae. In magnetoelectric materials, these degrees of freedom are closely coupled, allowing polarization to be controlled by a magnetic field, and magnetization by an electric field, but the magnitude of the effect remains a challenge in the case of single-phase magnetoelectrics for applications. We demonstrate that the magnetoelectric properties of the mixed-anisotropy antiferromagnet LiNi1−x Fe x PO4 are profoundly affected by partial substitution of Ni2+ ions with Fe2+ on the transition metal site. This introduces random site-dependent single-ion anisotropy energies and causes a lowering of the magnetic symmetry of the system. In turn, magnetoelectric couplings that are symmetry-forbidden in the parent compounds, LiNiPO4 and LiFePO4, are unlocked and the dominant coupling is enhanced by almost two orders of magnitude. Our results demonstrate the potential of mixed-anisotropy magnets for tuning magnetoelectric properties.

Abstract Magnetic topological insulators and semimetals are a class of crystalline solids whose properties are strongly influenced by the coupling between non-trivial electronic topology and magnetic spin configurations. Such materials can host exotic electromagnetic responses. Among these are topological insulators with certain types of antiferromagnetic order which are predicted to realize axion electrodynamics. Here we investigate the highly unusual helimagnetic phases recently reported in EuIn2As2, which has been identified as a candidate for an axion insulator. Using resonant elastic x-ray scattering we show that the two types of magnetic order observed in EuIn2As2 are spatially uniform phases with commensurate chiral magnetic structures, ruling out a possible phase-separation scenario, and we propose that entropy associated with low energy spin fluctuations plays a significant role in driving the phase transition between them. Our results establish that the magnetic order in EuIn2As2 satisfies the symmetry requirements for an axion insulator.

We examine the role of charge, structural, and spin degrees of freedom in the previously poorly understood phase transition in the 5d^{1} transition-metal double perovskite Cs_{2}TaCl_{6} using a combination of computational and experimental techniques. Our heat capacity measurements of single-crystalline Cs_{2}TaCl_{6} reveal a clear anomaly at the transition temperature, T_{Q}, which was not previously observed in polycrystalline samples. Density functional calculations indicate the emergence of local charge quadrupoles in the cubic phase, mediated by the paramagnetic spins or local structural distortions which then develop into long-range-ordered charge quadrupoles in the tetragonal phase. Our resonant elastic x-ray scattering on Cs_{2}TaCl_{6} single crystals lends support to our calculations. Our work provides insight into the phase transition in Cs_{2}TaCl_{6} at T_{Q}, and demonstrates the utility of this unique combination of techniques in understanding the complex physics of hidden orders in paramagnetic spin-orbit-entangled compounds.

We address magnetic neutron scattering in the presence of local noncentrosymmetric asymmetries of the magnetization density. Such inversion-symmetry breaking, combined with the absence of time-reversal symmetry, can be described in terms of magnetoelectric multipoles which form the second term after the magnetic dipole in the multipole expansion of the magnetization density. We provide a pedagogical review of the theoretical formalism of magnetic neutron diffraction in terms of the multipole expansion of the scattering cross-section. In particular, we show how to compute the contribution of magnetoelectric multipoles to the scattering amplitude starting from ab initio calculations. We also provide general guidelines on how to experimentally detect long-range order of magnetoelectric multipoles using either unpolarized or polarized neutron scattering. We apply the formalism to CuO, and we discuss first-principles predictions and experimental spherical neutron polarimetry measurements that are consistent with the presence of magnetoelectric multipoles in CuO.

We derive a compact matrix expression for the linear thermal expansion coefficients (TECs) for a general orthorhombic system which relates elastic properties and integrated quantities based on deformation and mode dependent Griineisen parameters and mode dependent heat capacities. The density of Griineisen parameters Γ(ν) as a function of frequency ν, weighted by the number of phonon modes, is introduced and found to be illuminating in interpreting the TEC results. Using density functional perturbation theory and Grüneisen formalism for thermal expansion, we illustrate the general usefulness of this method by calculating the linear and volumetric TECs of a low-symmetry orthorhombic compound antimony sulfide (Sb2S3), which belongs to a large class of technologically and fundamentally important materials. Even though negative Griineisen parameters are found for deformations in all three crystal directions, the Γ(ν) data rule out the occurrences of negative TECs at all temperatures. Sb2S3 exhibits a large thermal expansion anisotropy where the TEC in the b direction can reach as high as 13 x 10-6 K-1 at high temperatures, about two and seven times larger than the TECs in the c and a direction, respectively. Our work suggests a general and practical first-principles approach to calculate the thermal properties of other complicated low-symmetry systems. [ABSTRACT FROM AUTHOR]