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

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.
Authors:
 [1] ; ORCiD logo [2] ;  [2] ; ORCiD logo [1] ; ORCiD logo [2] ; ORCiD logo [1] ; ORCiD logo [2] ;  [1] ; ORCiD logo [1] ; ORCiD logo [2]
  1. Univ. of Antwerp, Antwerp (Belgium)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Report Number(s):
NREL/JA-5K00-71396
Journal ID: ISSN 1936-0851
Grant/Contract Number:
AC36-08GO28308
Type:
Published Article
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 12; Journal Issue: 7; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; carbon nanotubes; encapsulation; energy transfer; exciton dynamics; solar photoconversion; spectroscopy
OSTI Identifier:
1463365
Alternate Identifier(s):
OSTI ID: 1461372