Spin Vortex Crystal Order in Organic Triangular Lattice Compound

Abstract

Organic salts represent an ideal experimental playground for studying the interplay between magnetic and charge degrees of freedom, which has culminated in the discovery of several spin-liquid candidates, such as $\kappa$-(ET)$_2$Cu$_2$(CN)$_3$ ($\kappa$-Cu). Recent theoretical studies indicate the possibility of chiral spin liquids stabilized by ring-exchange, but the parent states with chiral magnetic order have not been observed in this material family. In this work, we discuss the properties of the recently synthesized $\kappa$-(BETS)$_2$Mn[N(CN)$_2$]$_3$ ($\kappa$-Mn). Based on analysis of specific heat, magnetic torque, and NMR measurements combined with ab initio calculations, we identify a spin-vortex crystal order. These observations definitively confirm the importance of ring-exchange in these materials, and support the proposed chiral spin-liquid scenario for triangular lattice organics.