Light-Programmable Logic-in-Memory in 2D Semiconductors Enabled by Supramolecular Functionalization: Photoresponsive Collective Effect of Aligned Molecular Dipoles

Nowadays, the unrelenting growth of the digital universe calls for radically novel strategies for data processing and storage. An extremely promising and powerful approach relies on the development of logic-in-memory (LiM) devices through the use of floating gate and ferroelectric technologies to write and erase data in a memory operating as a logic gate driven by electrical bias. In this work, we report an alternative approach to realize the logic-in-memory based on two-dimensional (2D) transition metal dichalcogenides (TMDs) where multiple memorized logic output states have been established via the interface with responsive molecular dipoles arranged in supramolecular arrays. The collective dynamic molecular dipole changes of the axial ligand coordinated onto self-assembled metal phthalocyanine nanostructures on the surface of 2D TMD enables large reversible modulation of the Fermi level of both n-type molybdenum disulfide (MoS2) and p-type tungsten diselenide (WSe2) field-effect transistors (FETs), to achieve multiple memory states by programming and erasing with ultraviolet (UV) and with visible light, respectively. As a result, logic-in-memory devices were built up with our supramolecular layer/2D TMD architecture where the output logic is encoded by the motion of the molecular dipoles. Our strategy relying on the dynamic control of the 2D electronics by harnessing the functions of molecular-dipole-induced memory in a supramolecular hybrid layer represents a versatile way to integrate the functional programmability of molecular science into the next generation nanoelectronics.