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.
| Original language | English |
|---|---|
| Pages (from-to) | 840-845 |
| Number of pages | 6 |
| Journal | Nature Chemistry |
| Volume | 5 |
| Issue number | 10 |
| DOIs | |
| Publication status | Published - Oct 2013 |
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ASJC Scopus subject areas
- Chemistry(all)
- Chemical Engineering(all)
Cite this
Brightening of carbon nanotube photoluminescence through the incorporation of sp 3 defects. / Piao, Yanmei; Meany, Brendan; Powell, Lyndsey R.; Valley, Nicholas; Kwon, Hyejin; Schatz, George C; Wang, Yuhuang.
In: Nature Chemistry, Vol. 5, No. 10, 10.2013, p. 840-845.Research output: Contribution to journal › Article
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TY - JOUR
T1 - Brightening of carbon nanotube photoluminescence through the incorporation of sp 3 defects
AU - Piao, Yanmei
AU - Meany, Brendan
AU - Powell, Lyndsey R.
AU - Valley, Nicholas
AU - Kwon, Hyejin
AU - Schatz, George C
AU - Wang, Yuhuang
PY - 2013/10
Y1 - 2013/10
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=84884844202&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84884844202&partnerID=8YFLogxK
U2 - 10.1038/nchem.1711
DO - 10.1038/nchem.1711
M3 - Article
C2 - 24056340
AN - SCOPUS:84884844202
VL - 5
SP - 840
EP - 845
JO - Nature Chemistry
JF - Nature Chemistry
SN - 1755-4330
IS - 10
ER -