This Telluride Science Research Center (TSRC) workshop will bring together experts in synthetic chemistry, theory and computation, spectroscopy, materials science and engineering, and device physics and engineering to scout the pathways forward to synthetically control the interfacial physicochemical response of organic semiconductors. Organic semiconductors, electronically and optically active materials derived from π-conjugated molecules and polymers, have been envisaged for use in a wide range of technologies, including transistors, solar cells, diode lighting and flexible displays, and bioelectronics. The potential for large-scale and low-cost device fabrication, distinctive device form factors that arise from the inherent mechanical flexibility of so-called ‘plastic’ materials, and the ability to readily tune the material electronic and optical properties through well-established chemical principles have driven the development, characterization, and device testing of thousands of organic materials. However, there remain numerous roadblocks to the widespread adoption of these materials, as critical links between the physicochemical processes that occur at the molecular scale and the behavior of the thin-film material under device operation have not been realized.

This limited understanding is particularly evident with regard to chemical and physical phenomena that occur when organic semiconductors come into contact with other materials, both organic and inorganic. Molecular packing in organic semiconductors is driven by relatively weak noncovalent interactions, and external forces greatly influence the structural heterogeneity that in turn dictates the electronic disorder that plagues these materials. While considerable effort has been put forward to synthetically design the bulk properties of organic semiconductors, there exist very few blueprints to govern the physicochemical processes that occur at the myriad interfaces in the broad application space envisioned. Ultimately, these limitations have left the community entwined in a spurious feedback loop that hinders the development of design principles to formulate materials with wide-ranging utility. Recent advances in synthesis, theory and computation, characterization, materials processing, and device design have positioned the community in a prime position to tackle issues that arise at the materials interface. This workshop will bring together expert voices from across a broad spectrum of disciplines to chart the next steps forward in the design of new generations of organic semiconductors with a view towards controlling interfacial chemical and physical phenomena.