Abstract
The Gadonanotubes (GNTs) are the highest-performing T1-weighted MRI contrast agent material known with a relaxivity of ∼160 mM−1s−1 per Gd3+ ion at 1.5 T. In this work, the contribution of carbon-based free radicals at defect sites on the sidewalls of the ultra-short carbon nanotube (US-tube) component of the GNTs to the T1 relaxation time has been investigated by Nuclear Magnetic Resonance Dispersion (NMRD) and Electron Paramagnetic Resonance (EPR) studies. The NMRD results indicate that carbon-based radicals of the US-tube structure substantially shorten water proton spin-lattice relaxation times at low frequencies (< 1 MHz) and that the high water proton relaxation rate for the GNTs at these fields does not result from the Gd3+ ion alone. Furthermore, a computational study suggests that the defect sites of the US-tube structure increase nanotube strain and create new interband electronic states. While the presence of Gd3+ ions at the defect sites for the GNTs do not induce new electronic states, they do introduce a shift in the Fermi level to higher energy (0.4 eV).
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