Ultrafast Charge and Exciton Diffusion in Monolayer Films of 9‐Armchair Graphene Nanoribbons

Abstract Determining the electronic transport properties of graphene nanoribbons is crucial for assessing their suitability for applications. So far, this has been highly challenging both through experimental and theoretical approaches. This is particularly the case for graphene nanoribbons that are prepared by chemical vapor deposition, which is a scalable and industry‐compatible bottom‐up growth method that results in closely packed arrays of ribbons with relatively short lengths of a few tens of nanometers. In this study, the experimental technique of spatiotemporal microscopy is applied to study monolayer films of 9‐armchair graphene nanoribbons prepared using this growth method, and combined with linear‐scaling quantum transport calculations of arrays of thousands of nanoribbons. Both approaches directly resolve electronic spreading in space and time through diffusion and give an initial diffusivity approaching 200 cm 2 s −1 during the first picosecond after photoexcitation. This corresponds to a mobility up to 550 cm 2 V −1 s −1 . The quasi‐free carriers then form excitons, which spread with a diffusivity of tens of cm 2 s −1 . The results indicate that this relatively large charge carrier mobility is the result of electronic transport not being hindered by defects nor inter‐ribbon hopping. This confirms their suitability for applications that require efficient electronic transport.