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The demand for high-density storage is urgent in the current era of dataexplosion. Recently, several single-molecule (-atom) magnets/ferroelectricshave been reported to be promising candidates for high-density storage. Asanother promising candidate, single-molecule multiferroics are not only smallbut also possess ferroelectric and magnetic orderings, which can sometimes bestrongly coupled and used as data storages to realize the combination ofelectric writing and magnetic reading. However, they have been rarely proposed,and never been experimentally reported. Here, by building Hamiltonian models,we propose a new model of single-molecule multiferroic in which electricdipoles and magnetic moments are parallel and can rotate with the rotation ofthe single molecule. Furthermore, with performing spin-lattice dynamicssimulations, we reveal the conditions (e.g., large enough single-ion anisotropyand appropriate electric field) under which the new single-moleculemultiferroic can arise. Based on this model, as well as first-principlescalculations, a realistic example Co(NH3)4N@SWCNT is constructed andnumerically confirmed to demonstrate the feasibility of the new single-moleculemultiferroic model. Our work not only sheds light on the discovery ofsingle-molecule multiferroics but also provides a new guideline to designmultifunctional materials for ultimate memory devices.

Towards Ultimate Memory with Single-Molecule Multiferroics