RESUMO
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)2Hg(SCN)2Br, 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. 1H 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.
RESUMO
Mott insulators are commonly pictured with electrons localized on lattice sites, with their low-energy degrees of freedom involving spins only. Here, we observe emergent charge degrees of freedom in a molecule-based Mott insulator κ-(BEDT-TTF)2Hg(SCN)2Br, resulting in a quantum dipole liquid state. Electrons localized on molecular dimer lattice sites form electric dipoles that do not order at low temperatures and fluctuate with frequency detected experimentally in our Raman spectroscopy experiments. The heat capacity and Raman scattering response are consistent with a scenario in which the composite spin and electric dipole degrees of freedom remain fluctuating down to the lowest measured temperatures.
RESUMO
We explore the nature of the metal-insulator transition in the two-dimensional organic compound ßâ³-(BEDT-TTF)2Hg(SCN)2Cl by x-ray, electrical transport, ESR, Raman, and infrared investigations. Magnetic and vibrational spectroscopy concurrently reveal a gradual dimerization along the stacking direction (a-b), setting in already at the crossover temperature of 150 K from the metallic to the insulating state. A spin gap of Δσ=47 meV is extracted. From the activated resistivity behavior below T = 55 K, a charge gap of Δρ=60 meV is derived. At TCO = 72 K, the C=C vibrational modes reveal the development of a charge-ordered state with a charge disproportionation of 2δρ=0.34e. In addition to a slight structural dimerization, charge-order causes stripes most likely perpendicular to the stacks.
RESUMO
According to band structure calculations, the Fermi surface of the quasi-two dimensional metal θ-(ET)4ZnBr4(C6H4Cl2) illustrates the linear chain of coupled orbits model. Accordingly, de Haas-van Alphen oscillations spectra recorded in pulsed magnetic field of up to 55 T evidence many Fourier components, the frequency of which are linear combinations of the frequencies relevant to the closed α and the magnetic breakdown ß orbits. The field and temperature dependence of their amplitude are quantitatively accounted for by analytic calculations including, beyond the Lifshitz-Kosevich formula, second-order terms in damping factors due to the oscillation of the chemical potential as the magnetic field varies. Whereas these second-order terms are negligible for the orbits α, ß and 2ß-α, they are solely responsible for the 'forbidden orbit' ß-α and its harmonic and have a significant influence on Fourier components such as 2α and ß+α, yielding strongly non-Lifshitz-Kosevich behaviour in the latter case.
