skip to main content


Title: Large off-diagonal magnetoelectricity in a triangular Co2+-based collinear antiferromagnet
Abstract

Magnetic toroidicity is an uncommon type of magnetic structure in solid-state materials. Here, we experimentally demonstrate that collinear spins in a material withR-3 lattice symmetry can host a significant magnetic toroidicity, even parallel to the ordered spins. Taking advantage of a single crystal sample of CoTe6O13with anR-3 space group and a Co2+triangular sublattice, temperature-dependent magnetic, thermodynamic, and neutron diffraction results reveal A-type antiferromagnetic order below 19.5 K, with magnetic point group -3′ andk = (0,0,0). Our symmetry analysis suggests that the missing mirror symmetry in the lattice could lead to the local spin canting for a toroidal moment along thecaxis. Experimentally, we observe a large off-diagonal magnetoelectric coefficient of 41.2 ps/m that evidences the magnetic toroidicity. In addition, the paramagnetic state exhibits a large effective moment per Co2+, indicating that the magnetic moment in CoTe6O13has a significant orbital contribution. CoTe6O13embodies an excellent opportunity for the study of next-generation functional magnetoelectric materials.

 
more » « less
NSF-PAR ID:
10477985
Author(s) / Creator(s):
; ; ; ; ; ; ; ;
Publisher / Repository:
Nature Publishing Group
Date Published:
Journal Name:
Nature Communications
Volume:
14
Issue:
1
ISSN:
2041-1723
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Quantum spin systems such as magnetic insulators usually show magnetic order, but such classical states can give way toquantum liquids with exotic entanglementthrough two known mechanisms of frustration: geometric frustration in lattices with triangle motifs, and spin-orbit-coupling frustration in the exactly solvable quantum liquid of Kitaev’s honeycomb lattice. Here we present the experimental observation of a new kind of frustrated quantum liquid arising in an unlikely place: the magnetic insulator Ba4Ir3O10where Ir3O12trimers form an unfrustrated square lattice. The crystal structure shows no apparent spin chains. Experimentally we find a quantum liquid state persisting down to 0.2 K that is stabilized by strong antiferromagnetic interaction with Curie–Weiss temperature ranging from −766 to −169 K due to magnetic anisotropy. The anisotropy-averaged frustration parameter is 2000, seldom seen in iridates. Heat capacity and thermal conductivity are both linear at low temperatures, a familiar feature in metals but here in an insulator pointing to an exotic quantum liquid state; a mere 2% Sr substitution for Ba produces long-range order at 130 K and destroys the linear-T features. Although the Ir4+(5d5) ions in Ba4Ir3O10appear to form Ir3O12trimers of face-sharing IrO6octahedra, we propose that intra-trimer exchange is reduced and the lattice recombines into an array of coupled 1D chains with additional spins. An extreme limit of decoupled 1D chains can explain most but not all of the striking experimental observations, indicating that the inter-chain coupling plays an important role in the frustration mechanism leading to this quantum liquid.

     
    more » « less
  2. Abstract

    Kagomé metals are widely recognized, versatile platforms for exploring topological properties, unconventional electronic correlations, magnetic frustration, and superconductivity. In theRV6Sn6family of materials (R= Sc, Y, Lu), ScV6Sn6hosts an unusual charge density wave ground state as well as structural similarities with theAV3Sb5system (A= K, Cs, Rb). In this work, we combine Raman scattering spectroscopy with first-principles lattice dynamics calculations to reveal phonon mixing processes in the charge density wave state of ScV6Sn6. In the low temperature phase, we find at least four new peaks in the vicinity of the V-containing totally symmetric mode near 240 cm−1suggesting that the density wave acts to mix modes ofP6/mmmand$$R\bar{3}m$$R3¯msymmetry - a result that we quantify by projecting phonons of the high symmetry state onto those of the lower symmetry structure. We also test the stability of the short-range ordered density wave state under compression and propose that both physical and chemical pressure quench the effect. We discuss these findings in terms of symmetry and the structure-property trends that can be unraveled in this system.

     
    more » « less
  3. Abstract

    Next‐generation electronics and energy technologies can now be developed as a result of the design, discovery, and development of novel, environmental friendly lead (Pb)‐free ferroelectric materials with improved characteristics and performance. However, there have only been a few reports of such complex materials’ design with multi‐phase interfacial chemistry, which can facilitate enhanced properties and performance. In this context, herein, novel lead‐free piezoelectric materials (1‐x)Ba0.95Ca0.05Ti0.95Zr0.05O3‐(x)Ba0.95Ca0.05Ti0.95Sn0.05O3, are reported, which are represented as (1‐x)BCZT‐(x)BCST, with demonstrated excellent properties and energy harvesting performance. The (1‐x)BCZT‐(x)BCST materials are synthesized by high‐temperature solid‐state ceramic reaction method by varyingxin the full range (x= 0.00–1.00). In‐depth exploration research is performed on the structural, dielectric, ferroelectric, and electro‐mechanical properties of (1‐x)BCZT‐(x)BCST ceramics. The formation of perovskite structure for all ceramics without the presence of any impurity phases is confirmed by X‐ray diffraction (XRD) analyses, which also reveals that the Ca2+, Zr4+, and Sn4+are well dispersed within the BaTiO3lattice. For all (1‐x)BCZT‐(x)BCST ceramics, thorough investigation of phase formation and phase‐stability using XRD, Rietveld refinement, Raman spectroscopy, high‐resolution transmission electron microscopy (HRTEM), and temperature‐dependent dielectric measurements provide conclusive evidence for the coexistence of orthorhombic + tetragonal (Amm2+P4mm) phases at room temperature. The steady transition ofAmm2crystal symmetry toP4mmcrystal symmetry with increasingxcontent is also demonstrated by Rietveld refinement data and related analyses. The phase transition temperatures, rhombohedral‐orthorhombic (TR‐O), orthorhombic‐ tetragonal (TO‐T), and tetragonal‐cubic (TC), gradually shift toward lower temperature with increasingxcontent. For (1‐x)BCZT‐(x)BCST ceramics, significantly improved dielectric and ferroelectric properties are observed, including relatively high dielectric constantεr≈ 1900–3300 (near room temperature),εr≈ 8800–12 900 (near Curie temperature), dielectric loss, tanδ≈ 0.01–0.02, remanent polarizationPr≈ 9.4–14 µC cm−2, coercive electric fieldEc≈ 2.5–3.6 kV cm−1. Further, high electric field‐induced strainS≈ 0.12–0.175%, piezoelectric charge coefficientd33≈ 296–360 pC N−1, converse piezoelectric coefficient ≈ 240–340 pm V−1, planar electromechanical coupling coefficientkp≈ 0.34–0.45, and electrostrictive coefficient (Q33)avg≈ 0.026–0.038 m4C−2are attained. Output performance with respect to mechanical energy demonstrates that the (0.6)BCZT‐(0.4)BCST composition (x= 0.4) displays better efficiency for generating electrical energy and, thus, the synthesized lead‐free piezoelectric (1‐x)BCZT‐(x)BCST samples are suitable for energy harvesting applications. The results and analyses point to the outcome that the (1‐x)BCZT‐(x)BCST ceramics as a potentially strong contender within the family of Pb‐free piezoelectric materials for future electronics and energy harvesting device technologies.

     
    more » « less
  4. Abstract

    BaZrO3(BZO) one-dimensional artificial pinning centers (1D-APCs) aligned along thec-axis of the YBa2Cu3O7(YBCO) have been adopted to enhance the magnetic vortex pinning in BZO/YBCO nanocomposite films. However, the pinning force densityFpof the BZO 1D-APCs remains moderate at temperatures near 77 K. A hypothesis of the major limiting factor is the defective BZO 1D-APCs/YBCO interface as a direct consequence of the large interfacial strain originated from the BZO/YBCO lattice mismatch of ∼7.7%. Herein, we explore enlarging thec-axis of the YBCO dynamically to reduce the lattice mismatch and hence to prevent formation of the defective BZO 1D-APCs/YBCO interface. Specifically, thec-axis enlargement was achieved by partial replacement of Cu with Ca on the YBCO lattice using strain-directed Ca diffusion into YBCO from two Ca0.3Y0.7Ba2Cu3O7x(CaY-123) spacers of only 10 nm in thickness inserted into the 2 vol% BZO 1D-APC/YBCO nanocomposite thin films of ∼150 nm in total thickness. The achieved elongatedc-axis is attributed to the formation of stacking faults induced by Ca-replacement of Cu on YBCO lattice. The reduced BZO/YBCO lattice mismatch allows formation of a coherent BZO 1D-APC/YBCO interface with negligible defects. This leads to an enhancedFpvalue up to 98 GN m−3at 65 K, which is 70% higher than that of the reference 2 vol% BZO 1D-APC/YBCO sample. Furthermore, the benefit of the enhanced pinning of the BZO 1D-APCs with a coherent interface with YBCO can be extended to a large angular range of the magnetic field orientation. This study reveals the significant effect of the BZO/YBCO interface on the pinning efficiency of BZO 1D-APCs and provides a promising approach to achieve a coherent interface in BZO/YBCO nanocomposite films.

     
    more » « less
  5. Abstract

    Large aqueous ions are interesting because they are useful in materials science (for example to generate thin films) but also because they serve as molecular models for the oxide–aqueous mineral interface where spectroscopy is difficult. Here we show that new clusters of the type M[(μ‐OH)2Co(NH3)4]3(NO3)6(M=Al, Ga) can be synthesized using Werner's century‐old cluster as a substitutable framework. We substituted Group 13 metals into the hexol Co[(μ‐OH)2Co(NH3)4]36+ion to make diamagnetic heterometallic ions. The solid‐state structure of the hexol‐type derivatives were determined by single‐crystal XRD and NMR spectroscopy and confirmed that the solid‐state structure persists in solution after dissolution into either D2O or [D6]DMSO. Other compositions besides these diamagnetic ions can undoubtedly be made using a similar approach, which considerably expands the number of stable aqueous heteronuclear ions.

     
    more » « less