Carbon nanobuds based on carbon nanotube caps: A first-principles study

TL;DR

This study uses first-principles calculations to show that fullerene C60 nanobuds form more favorably on carbon nanotube caps than on sidewalls, with implications for electronic properties and stability.

Contribution

It reveals that CNBs form more easily and are more stable on CNT caps, and explores their charge transport properties using advanced computational methods.

Findings

CNBs form more favorably on CNT caps than sidewalls.

The [2+2] cycloaddition is exothermic on caps, endothermic on sidewalls.

Charge transport shows resonant transmission and absence of quantum interference in CNT cap-C60 bonds.

Abstract

Based on density functional theory calculations, we here show that the formation of a fullerene C$_{60}$ carbon "nanobud" (CNB) on carbon nanotube (CNT) caps is energetically more favorable than that on CNT sidewalls. The dominant CNB formation mode for CNT caps is found to be the [2+2] cycloaddition reaction as in the conventional CNT sidewall case. However, it is identified to be exothermic in contrast to the endothermic reaction on CNT sidewalls. Computed reaction pathways further demonstrate that the formation (dissociation) barrier for the CNT cap-based CNB is slightly lower (significantly higher) than that of the CNT sidewall-based CNB, indicating an easier CNB formation as well as a higher structural stability. Additionally, performing matrix Green's function calculations, we study the charge transport properties of the CNB/metal electrode interfaces, and show that the C$_{60}$ bonding to the CNT cap or open end induces resonant transmissions near the Fermi level. It is also found that the good electronic linkage in the CNT cap-C$_{60}$ cycloaddition bonds results in the absence of quantum interference patterns, which contrasts the case of the CNB formed on an open-ended CNT that shows a Fano resonance profile.