Optical Identification of a DNA-Wrapped Carbon Nanotube: Signs of Helically Broken Symmetry

TL;DR

This study investigates how DNA wrapping alters the optical properties of single-walled carbon nanotubes, revealing significant changes such as circular dichroism, which could impact their use in optoelectronic devices.

Contribution

It provides the first analysis of DNA-induced optical property changes in SWNTs under perpendicular polarization, highlighting effects not seen in previous studies.

Findings

DNA wrapping causes strong circular dichroism in SWNTs.

Optical absorption spectra are qualitatively altered by DNA hybridization.

Changes are pronounced in perpendicular polarization geometry.

Abstract

High intrinsic mobility and small, biologically-compatible size make single-walled carbon nanotubes (SWNTs) in demand for the next generation of electronic devices. Further, the wide range of available bandgaps due to changes in diameter and symmetry give SWNTs greater versatility than traditional semiconductors. Single-stranded DNA has been employed to make these desirable properties accessible for large scale fabrication of devices. Because single-stranded DNA can helically wrap a SWNT, forming a stable hybrid structure, DNA/polymer wrapping has been used to disperse bundles of intrinsically hydrophobic SWNTs into individual tubes in aqueous solution. The ability to isolate individual tubes, make them soluble, and separate them according to symmetry would enable fabrication of SWNT optoelectronic devices that benefit from the unique electronic properties of specific nanotube structures. Envisioning optoelectronic applications of nanotubes, we investigate whether the optical properties of DNA-wrapped SWNT materials are different than those of pristine SWNTs. Our previous work found that bandstructures of DNA-SWNTs were indeed affected by the charged wrap. That is, the direct optical bandgap, $E_{11}$, decreases, but changes are fairly small. This is consistent with the available experimental data in standard experimental geometry in which incident light is polarized along the SWNT axis. Here we consider optical absorption of light with perpendicular (or circular) polarization with respect to the tube axis, which has been measured experimentally for SWNTs dispersed using a surfactant. In this geometry we find qualitative changes in the absorption spectra of SWNTs upon hybridization with DNA, including strong optical circular dichroism in non-chiral SWNTs.