Electron-Phonon Scattering Is Much Weaker in Carbon Nanotubes than in Graphene Nanoribbons

摘要

Carbon nanotubes (CNTs) and graphene nanoribbons (GNRs) are lower-dimensional derivatives of graphene. Similar to graphene, they exhibit high charge mobilities; howeVer, in contrast to graphene, they are semiconducting and thus are suitable for electronics, optics, solar energy devices, and other applications. Charge carrier mobilities, energies, and lifetimes are governed by scattering with phonons, and we demonstrate, using ab initio nonadiabatic molecular dynamics, that charge-phonon scattering is much stronger in GNRs. Focusing on a GNR and a CNT of similar size and electronic properties, we show that the difference arises because of the significantly higher stiffness of the CNT. The GNR undergoes large-scale undulating motions at ambient conditions. Such thermal geometry distortions localize wave functions, accelerate both elastic and inelastic charge-phonon scattering, and increase the rates of energy and carrier losses. Even though, formally, both CNTs and GNRs are quantum confined derivatives of graphene, charge-phonon scattering differs significantly between them. Showing good agreement with time-resolved photoconductivity and photoluminescence measurements, the study demonstrates that GNRs are quite similar to molecules, such as conjugated polymers, while CNTs exhibit extended features attributed to bulk materials. The state-of-the-art simulations alter the traditional view of graphene nanostructures and demonstrate that the performance can be tuned not only by size and composition but also by stiffness and response to thermal excitation.