Unconventional Magnetic and Resistive Hysteresis in an Iodine-Bonded Molecular Conductor†

Simultaneous manipulation of both spin and charge is a crucial issue in magnetic conductors. We report on a strong correlation between magnetism and conductivity in the iodine-bonded molecular conductor (DIETSe)2FeBr2Cl2 [DIETSe=diiodo(ethylenedithio)tetraselenafulvalene], which is the first molecular conductor showing a large hysteresis in both magnetic moment and magnetoresistance associated with a spin-flop transition. Utilizing a mixed-anion approach and iodine bonding interactions, we tailored a molecular conductor with random exchange interactions exhibiting unforeseen physical properties.