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Title: Photoluminescence imaging of solitary dopant sites in covalently doped single-wall carbon nanotubes

Abstract

Covalent dopants in semiconducting single wall carbon nanotubes (SWCNTs) are becoming important as routes for introducing new photoluminescent emitting states with potential for enhanced quantum yields, new functionality, and as species capable of near-IR room-temperature single photon emission. The origin and behavior of the dopant-induced emission is thus important to understand as a key requirement for successful room-T photonics and optoelectronics applications. Here, we use direct correlated two-color photoluminescence imaging to probe how the interplay between the SWCNT bright E 11 exciton and solitary dopant sites yields the dopant-induced emission for three different dopant species: oxygen, 4-methoxybenzene, and 4-bromobenzene. We introduce a route to control dopant functionalization to a low level as a means for introducing spatially well-separated solitary dopant sites. Resolution of emission from solitary dopant sites and correlation to their impact on E 11 emission allows confirmation of dopants as trapping sites for localization of E 11 excitons following their diffusive transport to the dopant site. Imaging of the dopant emission also reveals photoluminescence intermittency (blinking), with blinking dynamics being dependent on the specific dopant. Density functional theory calculations were performed to evaluate the stability of dopants and delineate the possible mechanisms of blinking. Furthermore, theoretical modeling suggestsmore » that the trapping of free charges in the potential well created by permanent dipoles introduced by dopant atoms/groups is likely responsible for the blinking, with the strongest effects being predicted and observed for oxygen-doped SWCNTs.« less

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1255120
Report Number(s):
LA-UR-15-28130
Journal ID: ISSN 2040-3364; NANOHL
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 7; Journal Issue: 48; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Hartmann, Nicolai F., Yalcin, Sibel Ebru, Adamska, Lyudmyla, Haroz, Erik H., Ma, Xuedan, Tretiak, Sergei, Htoon, Han, and Doorn, Stephen K. Photoluminescence imaging of solitary dopant sites in covalently doped single-wall carbon nanotubes. United States: N. p., 2015. Web. doi:10.1039/C5NR06343D.
Hartmann, Nicolai F., Yalcin, Sibel Ebru, Adamska, Lyudmyla, Haroz, Erik H., Ma, Xuedan, Tretiak, Sergei, Htoon, Han, & Doorn, Stephen K. Photoluminescence imaging of solitary dopant sites in covalently doped single-wall carbon nanotubes. United States. https://doi.org/10.1039/C5NR06343D
Hartmann, Nicolai F., Yalcin, Sibel Ebru, Adamska, Lyudmyla, Haroz, Erik H., Ma, Xuedan, Tretiak, Sergei, Htoon, Han, and Doorn, Stephen K. Wed . "Photoluminescence imaging of solitary dopant sites in covalently doped single-wall carbon nanotubes". United States. https://doi.org/10.1039/C5NR06343D. https://www.osti.gov/servlets/purl/1255120.
@article{osti_1255120,
title = {Photoluminescence imaging of solitary dopant sites in covalently doped single-wall carbon nanotubes},
author = {Hartmann, Nicolai F. and Yalcin, Sibel Ebru and Adamska, Lyudmyla and Haroz, Erik H. and Ma, Xuedan and Tretiak, Sergei and Htoon, Han and Doorn, Stephen K.},
abstractNote = {Covalent dopants in semiconducting single wall carbon nanotubes (SWCNTs) are becoming important as routes for introducing new photoluminescent emitting states with potential for enhanced quantum yields, new functionality, and as species capable of near-IR room-temperature single photon emission. The origin and behavior of the dopant-induced emission is thus important to understand as a key requirement for successful room-T photonics and optoelectronics applications. Here, we use direct correlated two-color photoluminescence imaging to probe how the interplay between the SWCNT bright E11 exciton and solitary dopant sites yields the dopant-induced emission for three different dopant species: oxygen, 4-methoxybenzene, and 4-bromobenzene. We introduce a route to control dopant functionalization to a low level as a means for introducing spatially well-separated solitary dopant sites. Resolution of emission from solitary dopant sites and correlation to their impact on E11 emission allows confirmation of dopants as trapping sites for localization of E11 excitons following their diffusive transport to the dopant site. Imaging of the dopant emission also reveals photoluminescence intermittency (blinking), with blinking dynamics being dependent on the specific dopant. Density functional theory calculations were performed to evaluate the stability of dopants and delineate the possible mechanisms of blinking. Furthermore, theoretical modeling suggests that the trapping of free charges in the potential well created by permanent dipoles introduced by dopant atoms/groups is likely responsible for the blinking, with the strongest effects being predicted and observed for oxygen-doped SWCNTs.},
doi = {10.1039/C5NR06343D},
url = {https://www.osti.gov/biblio/1255120}, journal = {Nanoscale},
issn = {2040-3364},
number = 48,
volume = 7,
place = {United States},
year = {2015},
month = {11}
}

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