By applying measurements of the dielectric constants and relative length changes to the dimerized molecular conductor κ-(BEDT-TTF)_{2}Hg(SCN)_{2}Cl, we provide evidence for order-disorder type electronic ferroelectricity that is driven by the charge order within the (BEDT-TTF)_{2} dimers and stabilized by a coupling to the anions. According to our density functional theory calculations, this material is characterized by a moderate strength of dimerization. This system thus bridges the gap between strongly dimerized materials, often approximated as dimer-Mott systems at 1/2 filling, and nondimerized or weakly dimerized systems at 1/4 filling, exhibiting a charge order. Our results indicate that intradimer charge degrees of freedom are of particular importance in correlated κ-(BEDT-TTF)_{2}X salts and can create novel states, such as electronically driven multiferroicity or charge-order-induced quasi-one-dimensional spin liquids.

This work shows an unconventional route for spin-driven ferroelectricity originating from a metastable magnetic field-induced canting of the chromium sublattice in the presence of gadolinium moments in GdCrTiO 5 at low temperatures. Compared to the isostructural neodymium compound, significant differences of magnetism and magnetoelectric effects are seen. We present the results of thorough investigations of temperature and magnetic field dependent magnetization as well as ac and dc magnetic susceptibility. These bulk measurements are complemented by local-probe spectroscopy utilizing electron-spin resonance and muon-spin rotation/relaxation for probing the chromium moments.Ferroelectric order is inferred from pyro-and magnetocurrent measurements. GdCrTiO 5 shows a pyrocurrent signal around 10 K, only if the system is cooled in an applied magnetic field exceeding 10 kOe. A distinct spin-driven ferroelectric order is revealed in this state for temperatures below 10 K, which can be switched by changing the magnetic-field direction and the polarity of the electric field. The magnetic measurements reveal no clear signature of long-range magnetic ordering. The presence of such 'meta-magnetoelectric-type' behaviour