Chirality Dependence of Triplet Excitons in (6,5) and (7,5) Single-Wall Carbon Nanotubes Revealed by Optically Detected Magnetic Resonance

Ivan Sudakov, Etienne Goovaerts, Wim Wenseleers, Jeffrey Blackburn, Juan Duque, Sofie Cambre

Research output: Contribution to journalArticlepeer-review

2 Scopus Citations

Abstract

The excitonic structure of single-wall carbon nanotubes (SWCNTs) is chirality dependent and consists of multiple singlet and triplet excitons (TEs) of which only one singlet exciton (SE) is optically bright. In particular, the dark TEs have a large impact on the integration of SWCNTs in optoelectronic devices, where excitons are created electrically, such as in infrared light-emitting diodes, thereby strongly limiting their quantum efficiency. Here, we report the characterization of TEs in chirality-purified samples of (6,5) and (7,5) SWCNTs, either randomly oriented in a frozen solution or with in-plane preferential orientation in a film, by means of optically detected magnetic resonance (ODMR) spectroscopy. In both chiral structures, the nanotubes are shown to sustain three types of TEs. One TE exhibits axial symmetry with zero-field splitting (ZFS) parameters depending on SWCNT diameter, in good agreement with the tighter confinement expected in narrower-diameter nanotubes. The ZFS of this TE also depends on nanotube environment, pointing to slightly weaker confinement for surfactant-coated than for polymer-wrapped SWCNTs. A second TE type, with much smaller ZFS, does not show the same systematic trends with diameter and environment and has a less well-defined axial symmetry. This most likely corresponds to TEs trapped at defect sites at low temperature, as exemplified by comparing SWCNT samples from different origins and after different treatments. A third triplet has unresolved ZFS, implying it originates from weakly interacting spin pairs. Aside from the diameter dependence, ODMR thus provides insights in both the symmetry, confinement, and nature of TEs on semiconducting SWCNTs.

Original languageAmerican English
Pages (from-to)2190-2204
Number of pages15
JournalACS Nano
Volume17
Issue number3
DOIs
StatePublished - 2023

Bibliographical note

Publisher Copyright:
© 2023 The Authors. Published by American Chemical Society.

NREL Publication Number

  • NREL/JA-5K00-83760

Keywords

  • angular dependence
  • chiral structure
  • optically detected magnetic resonance
  • single-wall carbon nanotubes
  • triplet excitons
  • zero-field splitting

Fingerprint

Dive into the research topics of 'Chirality Dependence of Triplet Excitons in (6,5) and (7,5) Single-Wall Carbon Nanotubes Revealed by Optically Detected Magnetic Resonance'. Together they form a unique fingerprint.

Cite this