Synthesis and Self-Assembly of Monodisperse Graphene Nanoribbons: Access to Submicron Architectures with Long-Range Order and Uniform Orientation

Fabricating organic semiconducting materials into large-scale, well-organized architectures is critical for building high-performance molecular electronics. While graphene nanoribbons (GNRs) hold enormous promise for various device applications, their assembly into a well-structured monolayer or multilayer architecture poses a substantial challenge. Here, we report the preparation of length-defined monodisperse GNRs via the integrated iterative binomial synthesis (IIBS) strategy and their self-assembly into submicrometer architectures with long-range order, uniform orientation, as well as regular layers. The use of short alkyl side chains benefits forming stable multilayers through interlocking structures. By changing the length and backbone shapes of these monodisperse GNRs, various three-dimensional assemblies, including multilayer stripes, monolayer stripes, and nanowires, can be achieved, leading to different photophysical properties and band gaps. The discovery of these intriguing self-assembly behaviors of length-defined GNRs is expected to enable various future applications.