Abstract
Electronic interactions in low-dimensional nanomaterial heterostructures can lead to novel optical responses arising from exciton delocalization over the constituent materials. Similar phenomena have been suggested to arise between closely interacting semiconducting carbon nanotubes of identical structure. Such behavior in carbon nanotubes has potential to generate new exciton physics, impact exciton transport mechanisms in nanotube networks, and place nanotubes as one-dimensional models for such behaviors in systems of higher dimensionality. Here we use resonance Raman spectroscopy to probe intertube interactions in (6,5) chirality-enriched bundles. Raman excitation profiles for the radial breathing mode and G-mode display a previously unobserved sharp resonance feature. We show the feature is evidence for creation of intertube excitons and is identified as a Fano resonance arising from the interaction between intratube and intertube excitons. The universality of the model suggests that similar Raman excitation profile features may be observed for interlayer exciton resonances in 2D multilayered systems.
Highlights
Electronic interactions in low-dimensional nanomaterial heterostructures can lead to novel optical responses arising from exciton delocalization over the constituent materials
Crochet et al.14 provided evidence of intertube excitons arising from tunneling of correlated electron-hole pairs between closely interacting singlewall carbon nanotube (SWCNT) within small bundles enriched in the [6,5] chirality
We find that specific [6,5]–(6,5) intertube interactions in such compositionally-defined bundles lead to the emergence of a previously unobserved sharp resonance feature that is superimposed on the intrinsic SWCNT Raman excitation profiles (REPs)
Summary
Electronic interactions in low-dimensional nanomaterial heterostructures can lead to novel optical responses arising from exciton delocalization over the constituent materials. Crochet et al. provided evidence of intertube excitons arising from tunneling of correlated electron-hole pairs between closely interacting SWCNTs within small bundles enriched in the [6,5] chirality This possibility expands the range of exciton physics in SWCNTs, while such compositionally-defined bundles are of growing interest in solar energy harvesting. We find that specific [6,5]–(6,5) intertube interactions in such compositionally-defined bundles lead to the emergence of a previously unobserved sharp resonance feature that is superimposed on the intrinsic SWCNT REP We show this sharp resonance (linewidth
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