Diameter-Dependent Optical Absorption and Excitation Energy Transfer from Encapsulated Dye Molecules toward Single-Walled Carbon Nanotubes

Jeffrey Blackburn, Rachelle Ihly, Andrew Ferguson, Justin Johnson, Stein Vezouw, Sofie Cambre, Jochen Campo, Joeri Defillet, Wim Wenseleers, Dylan Arias

Research output: Contribution to journalArticlepeer-review

35 Scopus Citations

Abstract

The hollow cores and well-defined diameters of single-walled carbon nanotubes (SWCNTs) allow for creation of one-dimensional hybrid structures by encapsulation of various molecules. Absorption and near-infrared photoluminescence-excitation (PLE) spectroscopy reveal that the absorption spectrum of encapsulated 1,3-bis[4-(dimethylamino)phenyl]-squaraine dye molecules inside SWCNTs is modulated by the SWCNT diameter, as observed through excitation energy transfer (EET) from the encapsulated molecules to the SWCNTs, implying a strongly diameter-dependent stacking of the molecules inside the SWCNTs. Transient absorption spectroscopy, simultaneously probing the encapsulated dyes and the host SWCNTs, demonstrates this EET, which can be used as a route to diameter-dependent photosensitization, to be fast (sub-picosecond). A wide series of SWCNT samples is systematically characterized by absorption, PLE, and resonant Raman scattering (RRS), also identifying the critical diameter for squaraine filling. In addition, we find that SWCNT filling does not limit the selectivity of subsequent separation protocols (including polyfluorene polymers for isolating only semiconducting SWCNTs and aqueous two-phase separation for enrichment of specific SWCNT chiralities). The design of these functional hybrid systems, with tunable dye absorption, fast and efficient EET, and the ability to remove all metallic SWCNTs by subsequent separation, demonstrates potential for implementation in photoconversion devices.

Original languageAmerican English
Pages (from-to)6881-6894
Number of pages14
JournalACS Nano
Volume12
Issue number7
DOIs
StatePublished - 2018

Bibliographical note

Publisher Copyright:
© 2018 American Chemical Society.

NREL Publication Number

  • NREL/JA-5K00-71396

Keywords

  • carbon nanotubes
  • encapsulation
  • energy transfer
  • exciton dynamics
  • solar photoconversion
  • spectroscopy

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