Crystallization-Mediated Magnetoelectric Response in Two-Dimensional Molecular Charge Transfer Crystals

Two-dimensional films and organic superstructures held by nonconvalent interaction with optoelectronic and magnetoelectric properties are of vital importance for sustainable energy and spintronics. Here, a bottom-up approach is proposed to organize tetrathiafulvalene and C60 into free-standing millimeter-sized single crystallized two-dimensional films by noncovalent charge transfer interactions. Opto-magnetoelectric properties of amorphous and crystallized films are compared. In addition, a high, broadband, and fast photoresponse from the UV to near-infrared region for the crystallized film is promising for flexible, lightweight photodetectors. The method proposed here is promising for scalable fabrication of other two-dimensional molecular films.