Broken symmetry optical transitions in (6,5) single-walled carbon nanotubes containing sp3 defects revealed by first-principles theory
Files
Accepted manuscript
Date
2024-01-17
Authors
Trerayapiwat, Kasidet Jing
Li, Xinxin
Ma, Xuedan
Sharifzadeh, Sahar
Version
Accepted manuscript
OA Version
Citation
K.J. Trerayapiwat, X. Li, X. Ma, S. Sharifzadeh. 2024. "Broken Symmetry Optical Transitions in (6,5) Single-Walled Carbon Nanotubes Containing sp3 Defects Revealed by First-Principles Theory." Nano Letters: a journal dedicated to nanoscience and nanotechnology, Volume 24, Issue 2, pp.667-671. https://doi.org/10.1021/acs.nanolett.3c03957
Abstract
We present a first-principles many-body perturbation theory study of nitrophenyl-doped (6,5) single-walled nanotubes (SWCNTs) to understand how sp3 doping impacts the excitonic properties. sp3-doped SWCNTs are promising as a class of optoelectronic materials with bright tunable photoluminescence, long spin coherence, and single-photon emission (SPE), motivating the study of spin excitations. We predict that the dopant results in a single unpaired spin localized around the defect site, which induces multiple low-energy excitonic peaks. By comparing optical absorption and photoluminescence from experiment and theory, we identify the transitions responsible for the red-shifted, defect-induced E11* peak, which has demonstrated SPE for some dopants; the presence of this state is due to both the symmetry-breaking associated with the defect and the presence of the defect-induced in-gap state. Furthermore, we find an asymmetry between the contribution of the two spin channels, suggesting that this system has potential for spin-selective optical transitions.