Quantum dipoles go liquid: Quantum spin liquids do not achieve an ordered magnetic state, even at the lowest temperatures. Hassan et al. studied an organic compound that may be both a spin liquid and a dipole liquid (see the Perspective by Powell). In the layered material κ-(BEDT-TTF) 2 Hg(SCN) 2 Br, molecules form charged dimers whose sites are arranged on a triangular lattice. The extra charge associated with each dimer can “live” on one of the two molecules in the dimer, resulting in a nonzero electric dipole moment for the dimer. Raman spectroscopy and heat capacity measurements revealed that, like spins in a quantum spin liquid, these dimers remained disordered down to the lowest temperatures. Science , this issue p. 1101 ; see also p. 1073
A new layered organic conductor θ-(BEDT-TTF)4CoBr4(1,2-C6H4Cl2) with different resistivity behaviour that has metallic conducting layers and is semiconducting perpendicular to the layers has been prepared. A phase transition near 320 K was found in this salt by temperature variable resistivity and X-ray diffraction measurements. Precise crystal structure data, below transition (triclinic phase) and above transition (tetragonal phase), was determined. The crystal structures of both phases are composed of θ-type radical cation layers alternating with layers involving [CoBr4]2− anions and 1,2-dichlorobenzene molecules. The lower symmetry in the crystal structure of the triclinic phase is due to a non-symmetrical arrangement of the solvent molecules within the anion layers. In each structure, the neighbouring conducting layers of the unit cell differ in stacking directions. In the tetragonal phase, all conducting layers are similar in structure, and in the low-temperature triclinic phase, the neighbouring conducting layers differ in periods along the stacks (4.703 Å and 4.993 Å) and in dihedral angles θ between the BEDT-TTF radical cations of the adjacent stacks. The finding of compounds of the θ-(BEDT-TTF)4CoBr4(1,2-C6H4Cl2) type with phase transitions above room temperature provides a wide possibility of investigating magnetoresistance, quantum oscillations, and the mechanism of interlayer transport in layered conductors.
We perform magnetic susceptibility and magnetic torque measurements on the organic κ-(BEDT-TTF)2Hg(SCN)2Br, which is recently suggested to host an exotic quantum dipole-liquid in its low-temperature insulating phase. Below the metal-insulator (MI) transition temperature, the magnetic susceptibility follows a Curie–Weiss law with a positive Curie–Weiss temperature, and a particular $$M\propto \sqrt{H}$$ curve is observed. The emergent ferromagnetically interacting spins amount to about 1/6 of the full spin moment of localized charges. Taking account of the possible inhomogeneous quasi-charge-order that forms a dipole-liquid, we construct a model of antiferromagnetically interacting spin chains in two adjacent charge-ordered domains, which are coupled via fluctuating charges on a Mott-dimer at the boundary. We find that the charge fluctuations can draw a weak ferromagnetic moment out of the spin singlet domains.
Mutual interactions in many-body systems bring about various exotic phases, among which liquid-like states failing to order due to frustration are of keen interest. The organic system with an anisotropic triangular lattice of molecular dimers, κ-(ET) 2 Hg(SCN) 2 Br, has been suggested to host a dipole liquid arising from intradimer charge-imbalance instability, possibly offering an unprecedented stage for the spin degrees of freedom. Here, we show that an extraordinary unordered/unfrozen spin state having soft matter–like spatiotemporal characteristics emerges in this system. 1 H nuclear magnetic resonance (NMR) spectra and magnetization measurements indicate that gigantic, staggered moments are nonlinearly and inhomogeneously induced by a magnetic field, whereas the moments vanish in the zero-field limit. The analysis of the NMR relaxation rate signifies that the moments fluctuate at a characteristic frequency slowing down to below megahertz at low temperatures. The inhomogeneity, local correlation, and slow dynamics indicative of middle-scale dynamical correlation length of several nanometers suggest novel frustration-driven spin clusterization.