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Brightening of carbon nanotube photoluminescence through the incorporation of sp3 defects
Abstract
Semiconducting carbon nanotubes promise a broad range of potential applications in optoelectronics and imaging, but their photon-conversion efficiency is relatively low. Quantum theory suggests that nanotube photoluminescence is intrinsically inefficient because of low-lying 'dark' exciton states. Here we demonstrate the significant brightening of nanotube photoluminescence (up to 28-fold) through the creation of an optically allowed defect state that resides below the predicted energy level of the dark excitons. Emission from this new state generates a photoluminescence peak that is red-shifted by as much as 254 meV from the nanotube's original excitonic transition. We also found that the attachment of electron-withdrawing substituents to carbon nanotubes systematically drives this defect state further down the energy ladder. Our experiments show that the material's photoluminescence quantum yield increases exponentially as a function of the shifted emission energy. This work lays the foundation for chemical control of defect quantum states in low-dimensional carbon materials.
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“Organic colour centres (OCCs) are molecularly tunable quantum defects on SWCNTs, which are produced by covalent functionalization of SWCNTs30,31.”
From Detection of ovarian cancer via the spectral fingerprinting of quantum-defect-modified carbon nanotubes in serum by machine learning (2022) · cites this paper as [31]
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Metadata
- Authors
- Piao, Y., Meany, B., Powell, L. R., Valley, N., Kwon, H., Schatz, G. C., & Wang, Y.
- Affiliations
- University of Maryland, College Park (US)
- Northwestern University (US)
- Corresponding author
- Wang, YuHuang
- Venue
- Nature Chemistry
- Published
- 2013-07-21
- Volume
- 5
- Issue
- 10
- Pages
- 840-845
- ISSN
- 1755-4330 (ISSN-L)
- 1755-4349
- OpenAlex
- W2007554685
- Cited by
- 480
- References
- 34
- Citations by year
- 2026: 33 · 2025: 41 · 2024: 44 · 2023: 43 · 2022: 41 · 2021: 43 · 2020: 32 · 2019: 43 · 2018: 41 · 2017: 38 · 2016: 39 · 2015: 24 · 2014: 17 · 2013: 1
- FWCI
- 12.18
- Type
- journal article
- Language
- en
- Open access
- closed
- Licence
- www.springer.com/tdm (tdm)
- Locations
- Nature Chemistry (publishedVersion)
- PubMed (publishedVersion)
- Funders
- Multidisciplinary University Research Initiative
- Army Research Office
- Topics
- Physical Sciences › Materials Science › Materials Chemistry › Graphene research and applications
- Physical Sciences › Materials Science › Materials Chemistry › Carbon Nanotubes in Composites
- Physical Sciences › Materials Science › Materials Chemistry › Carbon and Quantum Dots Applications
- Keywords
- carbon nanotubes, sp3 defects, defect states, dark excitons, red-shifted emission, electron-withdrawing substituents, photoluminescence quantum yield, single-walled carbon nanotubes, chemical functionalization, photon conversion efficiency
- MeSH terms
- Electrons, Luminescent Measurements, Particle Size, Quantum Theory, Nanotubes, Carbon
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