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Title: Low-Temperature Single Carbon Nanotube Spectroscopy of sp 3 Quantum Defects

Abstract

Aiming to unravel the relationship between chemical configuration and electronic structure of sp3 defects of aryl-functionalized (6,5) single-walled carbon nanotubes (SWCNTs), we perform low-temperature single nanotube photoluminescence (PL) spectroscopy studies and correlate our observations with quantum chemistry simulations. Here, we observe sharp emission peaks from individual defect sites that are spread over an extremely broad, 1000-1350 nm, spectral range. Our simulations allow us to attribute this spectral diversity to the occurrence of six chemically and energetically distinct defect states resulting from topological variation in the chemical binding configuration of the monovalent aryl groups. Both PL emission efficiency and spectral line width of the defect states are strongly influenced by the local dielectric environment. Wrapping the SWCNT with a polyfluorene polymer provides the best isolation from the environment and yields the brightest emission with near-resolution limited spectral line width of 270 ueV, as well as spectrally resolved emission wings associated with localized acoustic phonons. Pump-dependent studies further revealed that the defect states are capable of emitting single, sharp, isolated PL peaks over 3 orders of magnitude increase in pump power, a key characteristic of two-level systems and an important prerequisite for single-photon emission with high purity. Our findings point to themore » tremendous potential of sp3 defects in development of room temperature quantum light sources capable of operating at telecommunication wavelengths as the emission of the defect states can readily be extended to this range via use of larger diameter SWCNTs.« less

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [3];  [1]; ORCiD logo [4];  [5];  [5]; ORCiD logo [5]; ORCiD logo [3]; ORCiD logo [6]; ORCiD logo [1]; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Theoretical Division and Center for Nonlinear Studies; North Dakota State Univ., Fargo, ND (United States). Dept. of Chemistry and Biochemistry
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States). National Center for Photovoltaics. Chemical and Materials Science Center
  4. North Dakota State Univ., Fargo, ND (United States). Dept. of Chemistry and Biochemistry
  5. Stevens Inst. of Technology, Hoboken, NJ (United States). Dept. of Physics
  6. Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies, Theoretical Division and Center for Nonlinear Studies
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
OSTI Identifier:
1400371
Report Number(s):
NREL/JA-5900-70314
Journal ID: ISSN 1936-0851
Grant/Contract Number:
AC36-08GO28308; AC02-05CH11231; DMR-1506711; ECCS-MRI-1531237; CHE-1413614
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 11; Journal Issue: 11; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 77 NANOSCIENCE AND NANOTECHNOLOGY; carbon nanotubes; diazonium doping; electronic structure; exciton localization; photoluminescence

Citation Formats

He, Xiaowei, Gifford, Brendan J., Hartmann, Nicolai F., Ihly, Rachelle, Ma, Xuedan, Kilina, Svetlana V., Luo, Yue, Shayan, Kamran, Strauf, Stefan, Blackburn, Jeffrey L., Tretiak, Sergei, Doorn, Stephen K., and Htoon, Han. Low-Temperature Single Carbon Nanotube Spectroscopy of sp 3 Quantum Defects. United States: N. p., 2017. Web. doi:10.1021/acsnano.7b03022.
He, Xiaowei, Gifford, Brendan J., Hartmann, Nicolai F., Ihly, Rachelle, Ma, Xuedan, Kilina, Svetlana V., Luo, Yue, Shayan, Kamran, Strauf, Stefan, Blackburn, Jeffrey L., Tretiak, Sergei, Doorn, Stephen K., & Htoon, Han. Low-Temperature Single Carbon Nanotube Spectroscopy of sp 3 Quantum Defects. United States. doi:10.1021/acsnano.7b03022.
He, Xiaowei, Gifford, Brendan J., Hartmann, Nicolai F., Ihly, Rachelle, Ma, Xuedan, Kilina, Svetlana V., Luo, Yue, Shayan, Kamran, Strauf, Stefan, Blackburn, Jeffrey L., Tretiak, Sergei, Doorn, Stephen K., and Htoon, Han. 2017. "Low-Temperature Single Carbon Nanotube Spectroscopy of sp 3 Quantum Defects". United States. doi:10.1021/acsnano.7b03022.
@article{osti_1400371,
title = {Low-Temperature Single Carbon Nanotube Spectroscopy of sp 3 Quantum Defects},
author = {He, Xiaowei and Gifford, Brendan J. and Hartmann, Nicolai F. and Ihly, Rachelle and Ma, Xuedan and Kilina, Svetlana V. and Luo, Yue and Shayan, Kamran and Strauf, Stefan and Blackburn, Jeffrey L. and Tretiak, Sergei and Doorn, Stephen K. and Htoon, Han},
abstractNote = {Aiming to unravel the relationship between chemical configuration and electronic structure of sp3 defects of aryl-functionalized (6,5) single-walled carbon nanotubes (SWCNTs), we perform low-temperature single nanotube photoluminescence (PL) spectroscopy studies and correlate our observations with quantum chemistry simulations. Here, we observe sharp emission peaks from individual defect sites that are spread over an extremely broad, 1000-1350 nm, spectral range. Our simulations allow us to attribute this spectral diversity to the occurrence of six chemically and energetically distinct defect states resulting from topological variation in the chemical binding configuration of the monovalent aryl groups. Both PL emission efficiency and spectral line width of the defect states are strongly influenced by the local dielectric environment. Wrapping the SWCNT with a polyfluorene polymer provides the best isolation from the environment and yields the brightest emission with near-resolution limited spectral line width of 270 ueV, as well as spectrally resolved emission wings associated with localized acoustic phonons. Pump-dependent studies further revealed that the defect states are capable of emitting single, sharp, isolated PL peaks over 3 orders of magnitude increase in pump power, a key characteristic of two-level systems and an important prerequisite for single-photon emission with high purity. Our findings point to the tremendous potential of sp3 defects in development of room temperature quantum light sources capable of operating at telecommunication wavelengths as the emission of the defect states can readily be extended to this range via use of larger diameter SWCNTs.},
doi = {10.1021/acsnano.7b03022},
journal = {ACS Nano},
number = 11,
volume = 11,
place = {United States},
year = 2017,
month = 9
}

Journal Article:
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  • Metallic single wall carbon nanotube devices were characterized using low temperature transport measurements to study how the growth conditions affect defect formation in carbon nanotubes. Suspended carbon nanotube devices were grown in situ by a molecular beam growth method on a pair of catalyst islands located on opposing Au electrodes fabricated by electron beam lithography. The authors present experimental evidence that defect formation in carbon nanotubes, in addition to the well known growth temperature dependence, is also affected by the nature and the composition of the carbon growth gases.
  • The synthesis of single-wall carbon nanotubes by Nd:YAG laser vaporization of a graphite/(Ni, Co) target is investigated by laser-induced luminescence imaging and spectroscopy of Co atoms, C{sub 2} and C{sub 3} molecules, and clusters at 1000 degree sign C in flowing 500 Torr Ar. These laser-induced emission images under typical synthesis conditions show that the plume of vaporized material is segregated and confined within a vortex ring which maintains a {approx}1 cm3 volume for several seconds. Using time-resolved spectroscopy and spectroscopic imaging, the time for conversion of atomic and molecular species to clusters was measured for both carbon (200 {mu}s)more » and cobalt (2 ms). This rapid conversion of carbon to nanoparticles, combined with transmission electron microscopy analysis of the collected deposits, indicate that nanotube growth occurs over several seconds in a plume of mixed nanoparticles. By adjusting the time spent by the plume within the high-temperature zone using these in situ diagnostics, single-walled nanotubes of controlled length were grown at an estimated rate of 0.2 {mu}m/s. (c) 2000 American Institute of Physics.« less
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  • No abstract prepared.
  • The superiority of the electronic transport properties of single-walled carbon nanotube (SWNT) ropes over SWNT mats is verified from low temperature and frequency-dependent transport. The overall change of resistance versus in nanotube mats shows that 3D variable range hopping is the dominant conduction mechanism within the 2–300 K range. The magneto-resistance (MR) is found to be predominantly negative with a parabolic nature, which can also be described by the hopping model. Although the positive upturn of the MR at low temperatures establishes the contribution from quantum interference, the inherent quantum transport in individual tubes is suppressed at elevated temperatures. Therefore, tomore » minimize multi-channel effects from inter-tube interactions and other defects, two-terminal devices were fabricated from aligned SWNT (extracted from a mat) for low temperature transport as well as high-frequency measurements. In contrast to the mat, the aligned ropes exhibit step-like features in the differential conductance within the 80–300 K temperature range. The effects of plasmon propagation, unique to one dimension, were identified in electronic transport as a non-universal power-law dependence of the differential conductance on temperature and source-drain voltage. The complex impedance showed high power transmission capabilities up to 65 GHz as well as oscillations in the frequency range up to 30 GHz. The measurements suggest that aligned SWNT ropes have a realistic potential for high-speed device applications.« less