Control of both the regularity of a material ensemble and nanoscale architecture provides unique opportunities to develop novel thermoelectric applications based on 2D materials. As an example, the authors explore the electronic and thermal properties of functionalized graphene nanoribbons (GNRs) in the single-sheet and helical architectures using multiscale simulations. The results suggest that appropriate functionalization enables precise tuning of the doping density in a planar donor/acceptor GNR ensemble without the need to introduce an explicit dopant, which is critical to the optimization of power factor. In addition, the self-interaction between turns of a GNR may induce long-range disorder along the helical axis, which suppresses the thermal contribution from phonons with long wavelengths, leading to anomalous length independent phonon thermal transport in the quasi-1D system.
Keywords: 2D‐material; density functional theory; graphene nanoribbons; helical architectures; thermoelectric.