Semiconducting single-walled carbon nanotubes (S-SWCNTs) have direct band gaps
with a range of 0.5 to 2 eV depending on the SWCNT chirality. The photoluminescence
(PL) quantum efficiency and the carriers’ radiative lifetime have been previously
studied but neither of them have been confirmed due to the large variation resulting
from ensemble averaging, environmental effects, SWCNT defects, and SWCNT bundles.
For example, quantum efficiency was estimated to be 0.01% to 7% and radiative
lifetime was estimated or calculated to be 10 to 100 ns. In this thesis, we study absorption
cross section, PL quantum efficiency and exciton relaxation dynamics from
single air-suspended S-SWCNTs and extract “intrinsic” S-SWCNT properties.
The photo-excited carriers are electron-hole pairs (called excitons) in a SWCNT
due to the strong Coulomb interactions in the nm-scale system. We selected relatively
bright and less defected S-SWCNTs on our samples for investigation. For each SSWCNT,
the tube length, orientation, absorption and emission spectra were recorded.
Experimentally, we observed that PL from a single S-SWCNT increases linearly at
low excitation intensity (linear regime) and saturates at higher intensity (saturation
regime). We also studied the exciton relaxation dynamics on each S-SWCNT by
femtosecond excitation correlation (FEC) spectroscopy and resolved two relaxation
time constants which were independent of the excitation intensity. We compare the
simulation results based on a stochastic model to the experimental data and extract essential parameters including S-SWCNT unitless absorption coefficient (typically
0.02 to 0.06), PL quantum efficiency (typically 7 to 20 %) and exciton relaxation
time constants. We observed very fast nonlinear exciton-exciton annihilation rate (>(2 ps)^−1) in a typical 5 μm-long S-SWCNTs. The exciton dynamics were consistent
from 4 different S-SWCNTs in the saturation regime and the average total exciton
number per pulse per tube in this saturation regime ranges from 2 to 12.
Compared to past work, the results (PL saturation curves and FEC data) between
S-SWCNTs are very consistent which supports our belief that we are studying
“intrinsic properties”. We found a higher absorption coefficient, and higher PL quantum
efficiency of S-SWCNTs compared to previous work. We also observe very fast
nonlinear exciton-exciton annihilation in a relatively longer S-SWCNT and at lower
exciton numbers. / Thesis (Master, Physics, Engineering Physics and Astronomy) -- Queen's University, 2009-01-08 20:38:56.433
| Identifer | oai:union.ndltd.org:LACETR/oai:collectionscanada.gc.ca:OKQ.1974/1652 |
| Date | 12 January 2009 |
| Creators | XIAO, YEE-FANG |
| Contributors | Queen's University (Kingston, Ont.). Theses (Queen's University (Kingston, Ont.)) |
| Source Sets | Library and Archives Canada ETDs Repository / Centre d'archives des thèses électroniques de Bibliothèque et Archives Canada |
| Language | English, English |
| Detected Language | English |
| Type | Thesis |
| Format | 2304264 bytes, application/pdf |
| Rights | This publication is made available by the authority of the copyright owner solely for the purpose of private study and research and may not be copied or reproduced except as permitted by the copyright laws without written authority from the copyright owner. |
| Relation | Canadian theses |
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