Toward a Theoretical Roadmap for Organic Memristive Materials

Abstract: Neuromorphic computing aspires to overcome the intrinsic inefficiencies of von Neumann architectures by co-locating memory and computation in physical devices that emulate biological neurons and synapses. Memristive materials stand at the core of this paradigm, enabling non-volatile, history-dependent electronic responses. While inorganic oxides currently dominate the field, molecular and polymeric systems can offer untapped advantages in terms of chemical tunability, structural flexibility, low-cost processing, and biocompatibility. However, progress has been hindered by the absence of a theoretical framework able to rationalize how molecular structure translates into memristive function. Here, a multiscale computational perspective is presented, outlining how quantum chemistry and molecular dynamics, among other approaches, can be integrated into a coherent methodology to design next-generation organic memristors. Three mechanisms, ionic migration, redox-driven switching, and conduction interplay in chiral molecules are examined as representative routes toward molecular neuromorphic hardware. The opportunities and challenges associated with each mechanism are discussed, together with a view on how a theoretically guided roadmap can accelerate the emergence of chemically engineered synaptic materials.