Chemical Selection of Emission State Configuration in a Quantum Light Emitter
Ming Zheng, Geyou Ao, Stephen K. Doorn
Covalently-introduced photoluminescent sp3 defects generate new emitting states and dramatically expand optical functionality of single-wall carbon nanotubes, opening routes to enhanced imaging, photon upconversion, and room-temperature single photon emission at telecom wavelengths. A significant challenge in harnessing this potential is that the nominally simple reaction chemistry of nanotube functionalization introduces a broad diversity of emitting states. Precisely defining a narrow band of emission wavelengths necessitates constraining these states, which requires a remarkable selectivity in molecular binding configuration on the nanotube surface. We show here that such selectivity can be obtained for aryl binding through functionalization of so-called zigzag nanotube structures, achieving a three-fold narrowing in emission bandwidth. Accompanying DFT modeling reveals that the associated structural symmetry collapses the defect states to two degenerate configurations, thus limiting emission wavelengths to a single narrow band. We show this behavior can only result from a predominant selectivity for ortho binding configurations of the aryl groups on the nanotube lattice.
, Ao, G.
and Doorn, S.
Chemical Selection of Emission State Configuration in a Quantum Light Emitter, Nature Chemistry, [online], https://tsapps.nist.gov/publication/get_pdf.cfm?pub_id=925593
(Accessed December 3, 2023)