Transition from Diffusive to Superdiffusive Transport in Carbon Nanotube Networks via Nematic Order Control.

The one-dimensional confinement of quasiparticles in individual carbon nanotubes (CNTs) leads to extremely anisotropic electronic and optical properties. In a macroscopic ensemble of randomly oriented CNTs, this anisotropy disappears together with other properties that make them attractive for certain device applications. The question however remains if not only anisotropy but also other types of behaviors are suppressed by disorder. Here, we compare the dynamics of quasiparticles under strong electric fields in aligned and random CNT networks using a combination of terahertz emission and photocurrent experiments and out-of-equilibrium numerical simulations. We find that the degree of alignment strongly influences the excited quasiparticles' dynamics, rerouting the thermalization pathways. This is, in particular, evidenced in the high-energy, high-momentum electronic population (probed through the formation of low energy excitons via exciton impact ionization) and the transport regime evolving from diffusive to superdiffusive.

Terahertz Excitonics in Carbon Nanotubes: Exciton Autoionization and Multiplication.

Excitons play major roles in optical processes in modern semiconductors, such as single-wall carbon nanotubes (CNTs), transition metal dichalcogenides, and 2D perovskite quantum wells. They possess extremely large binding energies (>100 meV), dominating absorption and emission spectra even at high temperatures. The large binding energies imply that they are stable, that is, hard to ionize, rendering them seemingly unsuited for optoelectronic devices that require mobile charge carriers, especially terahertz emitters and solar cells. Here, we have conducted terahertz emission and photocurrent studies on films of aligned single-chirality semiconducting CNTs and find that excitons autoionize, i.e., spontaneously dissociate into electrons and holes. This process naturally occurs ultrafast (<1 ps) while conserving energy and momentum. The created carriers can then be accelerated to emit a burst of terahertz radiation when a dc bias is applied, with promising efficiency in comparison to standard GaAs-based emitters. Furthermore, at high bias, the accelerated carriers acquire high enough kinetic energy to create secondary excitons through impact exciton generation, again in a fully energy and momentum conserving fashion. This exciton multiplication process leads to a nonlinear photocurrent increase as a function of bias. Our theoretical simulations based on nonequilibrium Boltzmann transport equations, taking into account all possible scattering pathways and a realistic band structure, reproduce all of our experimental data semiquantitatively. These results not only elucidate the momentum-dependent ultrafast dynamics of excitons and carriers in CNTs but also suggest promising routes toward terahertz excitonics despite the orders-of-magnitude mismatch between the exciton binding energies and the terahertz photon energies.