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

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.

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]
+ Show Author Affiliations
  1. Physics Department, University of Antwerp, Universiteitsplein 1, B-2610 Antwerp, Belgium
  2. Chemistry & Nanoscience Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States
Publication Date:
Research Org.:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1463365
Alternate Identifier(s):
OSTI ID: 1461372; OSTI ID: 1508594
Report Number(s):
NREL/JA-5K00-71396
Journal ID: ISSN 1936-0851
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Published Article
Journal Name:
ACS Nano
Additional Journal Information:
Journal Name: ACS Nano Journal Volume: 12 Journal Issue: 7; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society
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

Citation Formats

van Bezouw, Stein, Arias, Dylan H., Ihly, Rachelle, Cambré, Sofie, Ferguson, Andrew J., Campo, Jochen, Johnson, Justin C., Defillet, Joeri, Wenseleers, Wim, and Blackburn, Jeffrey L. Diameter-Dependent Optical Absorption and Excitation Energy Transfer from Encapsulated Dye Molecules toward Single-Walled Carbon Nanotubes. United States: N. p., 2018. Web. doi:10.1021/acsnano.8b02213.
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van Bezouw, Stein, Arias, Dylan H., Ihly, Rachelle, Cambré, Sofie, Ferguson, Andrew J., Campo, Jochen, Johnson, Justin C., Defillet, Joeri, Wenseleers, Wim, & Blackburn, Jeffrey L. Diameter-Dependent Optical Absorption and Excitation Energy Transfer from Encapsulated Dye Molecules toward Single-Walled Carbon Nanotubes. United States. https://doi.org/10.1021/acsnano.8b02213
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van Bezouw, Stein, Arias, Dylan H., Ihly, Rachelle, Cambré, Sofie, Ferguson, Andrew J., Campo, Jochen, Johnson, Justin C., Defillet, Joeri, Wenseleers, Wim, and Blackburn, Jeffrey L. Mon . "Diameter-Dependent Optical Absorption and Excitation Energy Transfer from Encapsulated Dye Molecules toward Single-Walled Carbon Nanotubes". United States. https://doi.org/10.1021/acsnano.8b02213.
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@article{osti_1463365,
title = {Diameter-Dependent Optical Absorption and Excitation Energy Transfer from Encapsulated Dye Molecules toward Single-Walled Carbon Nanotubes},
author = {van Bezouw, Stein and Arias, Dylan H. and Ihly, Rachelle and Cambré, Sofie and Ferguson, Andrew J. and Campo, Jochen and Johnson, Justin C. and Defillet, Joeri and Wenseleers, Wim and Blackburn, Jeffrey L.},
abstractNote = {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.},
doi = {10.1021/acsnano.8b02213},
journal = {ACS Nano},
number = 7,
volume = 12,
place = {United States},
year = {Mon Jul 02 00:00:00 EDT 2018},
month = {Mon Jul 02 00:00:00 EDT 2018}
}
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https://doi.org/10.1021/acsnano.8b02213
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