LAUSR

Abstract It is known that an isolated single‐molecule magnet tends to become super‐paramagnetic even at an ultralow temperature of a few Kelvin due to the low spin switching barrier. Herein, single‐molecule ferroelectrics/multiferroics is proposed, as the ultimate size limit of memory, such that every molecule can store 1 bit data. The primary strategy is to identify polar molecules that possess bistable states, moderate switching barriers, and polarizations fixed along the vertical direction for high‐density perpendicular recording. First‐principles computation shows that several selected magnetic metal porphyrin molecules possess buckled structures with switchable vertical polarizations that are robust at ambient conditions. When intercalated within a bilayer of 2D materials such as bilayer MoS2 or CrI3, the magnetization can alter the spin distribution or can be even switched by 180° upon ferroelectric switching, rendering efficient electric writing and magnetic reading. It is found that the upper limit of areal storage density can be enhanced by four orders of magnitude, from the previous super‐paramagnetic limit of ≈40 to ≈106 GB in.−2, on the basis of the design of cross‐point multiferroic tunneling junction array and multiferroic hard drive.