Providing Time to Transfer: Longer Lifetimes Lead to Improved Energy Transfer in Films of Semiconducting Carbon Nanotubes.

The performance of photovoltaic devices made using semiconducting carbon nanotubes is limited by the transverse exciton diffusion length, which is ultimately set by intertube energy transfer. In this paper, we study whether extending the exciton lifetime improves energy transfer, by allowing more time for exciton transfer between carbon nanotubes, and thereby device performance. To do so, we prepare nanotubes by either shear-force mixing or ultrasonication, leading to different lengths and defect densities. We create thin films that mix (6,5) and (7,5) nanotubes and quantify the relative amounts of energy transfer in them using two-dimensional white-light (2DWL) spectroscopy and photoluminescence excitation (PLE) spectroscopy. Cross-peaks appearing in 2DWL spectra and quenching of the (6,5) PLE signal upon mixing both quantify energy transfer from (6,5) to (7,5). In both spectroscopies, energy transfer between shear-force mixed tubes is ∼20% more efficient. The cross-peaks in 2DWL spectra grow in at the same rate regardless of the processing method with the all shear-force mixed sample ultimately reaching a larger cross-peak amplitude. Shear-force mixing methods instead of sonication have improved external quantum efficiency in carbon nanotube devices by 30%. The spectroscopic results observed here link energy transfer to exciton diffusion and correlate to device performance.