First-passage theory of exciton population loss in single-walled carbon nanotubes reveals micron-scale intrinsic diffusion lengths

Abstract: One-dimensional crystals have long range translational invariance which manifests as long exciton diffusion lengths, but such intrinsic properties are often obscured by environmental perturbations. We use a first-passage approach to model single-walled carbon nanotube (SWCNT) exciton dynamics (including exciton-exciton annihilation and end effects) and compare it to results from both continuous-wave and multi-pulse ultrafast excitation experiments to extract intrinsic SWCNT properties. Excitons in suspended SWCNTs experience macroscopic diffusion lengths, on the order of the SWCNT length, (1.3-4.7 um) in sharp contrast to encapsulated samples. For these pristine samples, our model reveals intrinsic lifetimes (350-750 ps), diffusion constants (130-350 cm^2/s), and absorption cross-sections (2.1-3.6 X 10^-17 cm^2/atom) among the highest previously reported.and diffusion lengths for SWCNTs.