How to recognize clustering of luminescent defects in single-wall carbon nanotubes

Semiconducting single-wall carbon nanotubes (SWCNTs) are a promising material platform for near-infrared in vivo imaging, optical sensing, and single-photon emission at telecommunication wavelengths. The functionalization of SWCNTs with luminescent defects can lead to significantly enhanced photolum...

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Hauptverfasser: Sebastian, Finn (VerfasserIn) , Settele, Simon (VerfasserIn) , Li, Han (VerfasserIn) , Flavel, Benjamin S. (VerfasserIn) , Zaumseil, Jana (VerfasserIn)
Dokumenttyp: Article (Journal)
Sprache:Englisch
Veröffentlicht: 03 Oct 2024
In: Nanoscale horizons
Year: 2024, Jahrgang: 9, Heft: 12, Pages: 2286-2294
ISSN:2055-6764
DOI:10.1039/D4NH00383G
Online-Zugang:Verlag, kostenfrei, Volltext: https://doi.org/10.1039/D4NH00383G
Verlag, kostenfrei, Volltext: https://pubs.rsc.org/en/content/articlelanding/2024/nh/d4nh00383g
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Verfasserangaben:Finn L. Sebastian, Simon Settele, Han Li, Benjamin S. Flavel and Jana Zaumseil

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520 |a Semiconducting single-wall carbon nanotubes (SWCNTs) are a promising material platform for near-infrared in vivo imaging, optical sensing, and single-photon emission at telecommunication wavelengths. The functionalization of SWCNTs with luminescent defects can lead to significantly enhanced photoluminescence (PL) properties due to efficient trapping of highly mobile excitons and red-shifted emission from these trap states. Among the most studied luminescent defect types are oxygen and aryl defects that have largely similar optical properties. So far, no direct comparison between SWCNTs functionalized with oxygen and aryl defects under identical conditions has been performed. Here, we employ a combination of spectroscopic techniques to quantify the number of defects, their distribution along the nanotubes and thus their exciton trapping efficiencies. The different slopes of Raman D/G+ ratios versus calculated defect densities from PL quantum yield measurements indicate substantial dissimilarities between oxygen and aryl defects. Supported by statistical analysis of single-nanotube PL spectra at cryogenic temperatures they reveal clustering of oxygen defects. The clustering of 2-3 oxygen defects, which act as a single exciton trap, occurs irrespective of the functionalization method and thus enables the use of simple equations to determine the density of oxygen defects and defect clusters in SWCNTs based on standard Raman spectroscopy. The presented analytical approach is a versatile and sensitive tool to study defect distribution and clustering in SWCNTs and can be applied to any new functionalization method. 
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