Charge and spin interplay in a molecular-dimer-based organic Mott insulator

Abstract

Triangular lattice quasi-two-dimensional Mott insulators based on BEDT-TTF molecule and its analogies present a possibility to produce exotic phases by coupling charge and spin degrees of freedom. In this work we discuss magnetic properties of one of such materials, $\kappa$-(BEDT-TTF)$_2$Hg(SCN)$_2$Cl, which is found at the border of the phase transition between a Mott insulator into a charge ordered state. Our magnetic susceptibility and cantilever magnetisation measurements demonstrate how the charge degree of freedom defines magnetic properties for few different charge phases observed in this material as a function of temperature. Between $T_{CO}=30~K$ and $T_S=24~K$ we observe charge and spin separation due to one-dimensional charge stripes formed in this material below $T_{CO}=30~K$. Below $T_S=24~K$ charge and spin degrees of freedom demonstrate coupling. Spin singlet correlations develop below 24~K, however melting of charge order below 15~K prevents the spin singlet state formation, leaving the system in the inhomogeneous state with charge ordered spin singlet domains and charge and spin fluctuating ones.