Electrically switchable magnetic and electronic properties are promising for quantum sensing and information technology. Here, we report an electrically driven magnetic and electronic phase transition in molecular electronic crystal, potassium-7,7,8,8-tetracyanoquinodimethan, with the magneto-electric switching over 105 cycles at room temperature. Electron spin resonance study reveals the cooperative transition between spin and charge degrees of freedom. In addition, the mechanistic spectroscopy studies suggest the charges in an inhomogeneous conductor-insulator mixed state. The findings shown here suggest electrically controlled ordering in strongly correlated molecular crystal leads to dynamic magneto-electric switching, paving the way for developing molecular-based memory and switching devices.
Keywords: dimerization; magneto-electric switching; magnetodielectric; magnetoresistance; molecular electronic crystal.