Toward Highly Robust Nonvolatile Multilevel Memory by Fine Tuning of the Nanostructural Crystalline Solid-State Order

Organic resistive memory (ORM) offers great promise for next-generation high-density multilevel-cell (MLC) data storage. However, the fine tuning of crystalline order among its active layer still remains challenging, which largely restricts ORM behavior. Here, an exceptional solid-state transition from disordered orientations to highly-uniform orientation within the ORM layer is facilely triggered via molecular strategic tailoring. Two diketopyrrolopyrrole-based small molecular analogues (NI₁TDPP and NI₂TDPP) are demonstrated to display different symmetry. The asymmetric NI₁TDPP shows an irregular solid-state texture, while the centro-symmetric NI₂TDPP conforms to an ordered out-of-plane single-crystalline pattern that aligns with the foremost charge transportation along the substrate normal, and exhibits excellent MLC memory characteristics. Moreover, this highly oriented pattern guarantees the large-area film uniformity, leading to the twofold increase in the yield of as-fabricated ORM devices. This study reveals that the solid-state crystalline nanostructural order of organic materials can be controlled by reasonable molecular design to actuate high-performance organic electronic circuits.