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Title: Multi-exciton emission from solitary dopant states of carbon nanotubes

Abstract

By separating the photons from slow and fast decays of single and multi-exciton states in a time gated 2nd order photon correlation experiment, we show that solitary oxygen dopant states of single-walled carbon nanotubes (SWCNTs) allow emission of photon pairs with efficiencies as high as 44% of single exciton emission. Here, our pump dependent time resolved photoluminescence (PL) studies further reveal diffusion-limited excitonโ€“exciton annihilation as the key process that limits the emission of multi-excitons at high pump fluences. We further postulate that creation of additional permanent exciton quenching sites occurring under intense laser irradiation leads to permanent PL quenching. With this work, we bring out multi-excitonic processes of solitary dopant states as a new area to be explored for potential applications in lasing and entangled photon generation.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2];  [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]
  1. Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
  2. Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1673361
Report Number(s):
LA-UR-18-29325
Journal ID: ISSN 2040-3364
Grant/Contract Number:  
89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 9; Journal Issue: 42; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; Material Science

Citation Formats

Ma, Xuedan, Hartmann, Nicolai F., Velizhanin, Kirill A., Baldwin, Jon Kevin Scott, Adamska, Lyudmyla, Tretiak, Sergei, Doorn, Stephen K., and Htoon, Han. Multi-exciton emission from solitary dopant states of carbon nanotubes. United States: N. p., 2017. Web. doi:10.1039/c7nr06661a.
Ma, Xuedan, Hartmann, Nicolai F., Velizhanin, Kirill A., Baldwin, Jon Kevin Scott, Adamska, Lyudmyla, Tretiak, Sergei, Doorn, Stephen K., & Htoon, Han. Multi-exciton emission from solitary dopant states of carbon nanotubes. United States. https://doi.org/10.1039/c7nr06661a
Ma, Xuedan, Hartmann, Nicolai F., Velizhanin, Kirill A., Baldwin, Jon Kevin Scott, Adamska, Lyudmyla, Tretiak, Sergei, Doorn, Stephen K., and Htoon, Han. Thu . "Multi-exciton emission from solitary dopant states of carbon nanotubes". United States. https://doi.org/10.1039/c7nr06661a. https://www.osti.gov/servlets/purl/1673361.
@article{osti_1673361,
title = {Multi-exciton emission from solitary dopant states of carbon nanotubes},
author = {Ma, Xuedan and Hartmann, Nicolai F. and Velizhanin, Kirill A. and Baldwin, Jon Kevin Scott and Adamska, Lyudmyla and Tretiak, Sergei and Doorn, Stephen K. and Htoon, Han},
abstractNote = {By separating the photons from slow and fast decays of single and multi-exciton states in a time gated 2nd order photon correlation experiment, we show that solitary oxygen dopant states of single-walled carbon nanotubes (SWCNTs) allow emission of photon pairs with efficiencies as high as 44% of single exciton emission. Here, our pump dependent time resolved photoluminescence (PL) studies further reveal diffusion-limited excitonโ€“exciton annihilation as the key process that limits the emission of multi-excitons at high pump fluences. We further postulate that creation of additional permanent exciton quenching sites occurring under intense laser irradiation leads to permanent PL quenching. With this work, we bring out multi-excitonic processes of solitary dopant states as a new area to be explored for potential applications in lasing and entangled photon generation.},
doi = {10.1039/c7nr06661a},
journal = {Nanoscale},
number = 42,
volume = 9,
place = {United States},
year = {Thu Oct 12 00:00:00 EDT 2017},
month = {Thu Oct 12 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Figures / Tables:

Fig. 1 Fig. 1: PL spectra (a, d), g(2) trace of all the photons (top trace) and time gated g(2) traces extracted at the gate delay time (TGD) indicated in the figures (b, e) (See SI. Fig. 1S for g(2) traces with time delay extending to 300 ns). PL decay curves (blue,more » right axis) and center to side peak area ratio (R) vs TGD plot (left axis) (c, f) for two doped SWCNTs. Black solid lines are guides to the eye. The data for (a-c) and (d-f) were acquired at 4 K and 200 K, respectively.« less

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Works referencing / citing this record:

Exciton relaxation in carbon nanotubes via electronic-to-vibrational energy transfer
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Figures / Tables found in this record:

    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.