sp³-Functionalization of Single-Walled Carbon Nanotubes Creates Localized Spins

Chemical functionalization-introduced sp³ quantum defects in single-walled carbon nanotubes (SWCNTs) have shown compelling optical properties for their potential applications in quantum information science and bioimaging. Here, we utilize temperature- and power-dependent electron spin resonance measurements to study the fundamental spin properties of SWCNTs functionalized with well-controlled densities of sp³ quantum defects. Signatures of isolated spins that are highly localized at the sp³ defect sites are observed, which we further confirm with density functional theory calculations. Applying temperature-dependent line width analysis and power-saturation measurements, we estimate the spin-lattice relaxation time T₁ and spin dephasing time T₂ to be around 9 μs and 40 ns, respectively. These findings of the localized spin states that are associated with the sp³ quantum defects not only deepen our understanding of the molecular structures of the quantum defects but could also have strong implications for their applications in quantum information science.