Magnetic response of carbon nanotubes from ab initio calculations

TL;DR

This paper uses ab initio calculations to study the magnetic susceptibility and chemical shifts of carbon nanotubes, revealing diameter and chirality dependencies and explaining experimental observations.

Contribution

It introduces a gauge-including projector augmented-wave method for magnetic response calculations in periodic systems, applied to semiconducting zigzag nanotubes.

Findings

Susceptibility and shift depend on diameter and chirality.

Isotropic shift follows an asymptotic formula with diameter.

Inner tube shifts are affected by outer tube's demagnetizing currents.

Abstract

We present {\it ab initio} calculations of the magnetic susceptibility and of the $^{13}$C chemical shift for carbon nanotubes, both isolated and in bundles. These calculations are performed using the recently proposed gauge-including projector augmented-wave approach for the calculation of magnetic response in periodic insulating systems. We have focused on the semiconducting zigzag nanotubes with diameters ranging from 0.6 to 1.6 nm. Both the susceptibility and the isotropic shift exhibit a dependence with the diameter (D) and the chirality of the tube (although this dependence is stronger for the susceptibility). The isotropic shift behaves asymptotically as $\alpha/D + 116.0$, where $\alpha$ is a different constant for each family of nanotubes. For a tube diameter of around 1.2 nm, a value normally found in experimental samples, our results are in excellent agreement with experiments. Moreover, we calculated the chemical shift of a double-wall tube. We found a diamagnetic shift of the isotropic lines corresponding to the atoms of the inner tube due to the effect of the outer tube. This shift is in good agreement with recent experiments, and can be easily explained by demagnetizing currents circulating the outer tube.