Diameter dependence of interwall separation and strain in multiwalled carbon nanotubes probed by X-ray diffraction and Raman scattering studies

摘要

We have made a systematic study on the diameter dependent spectral features in X-ray diffraction (XRD) and Raman scattering studies of multiwalled carbon nanotubes (MWCNTs) of various diameters in the range 5-100 nm. High resolution transmission electron microscopy (HRTEM) imaging reveals a systematic decrease in the interwall separation from 3.8 A down to 3.2 A as the diameter of nanotubes increases from 5.8 nm to 63.2 nm. Analysis of the XRD patterns shows an exponential decrease in d002 interlayer spacing with increasing tube diameter, in close agreement with the HRTEM results. Further, XRD profile line width shows inverse diameter dependence and exponential increase in intensity as the diameter of the MWCNTs increases. Raman spectra of different diameter nanotubes show different evolutions of metallic and semiconducting components in the G-band, as found from spectral deconvolution. The frequency and full width at half maximum (FWHM) of the semiconducting component of the G~- band gradually decreases as the tube diameter increases. Ratio of intensities of G~- band to D-band first shows a sharp fall as the tube diameter increases from 7 nm to 15 nm and then slowly increases with increasing diameter. On the other hand, Gmode frequency shows large up shift when average diameter is increased from 7 nm to 15 nm and then saturates for higher diameter tubes. Analysis of Raman and XRD data reveals that the lowest diameter (7 nm) MWCNTs have features similar to those of the single walled nanotubes, while the spectral features are distinctly different for higher diameter MWCNTs due to the interaction among tube walls that is very significant for large diameter MWCNTs. Observed diameter dependence of the spectral features is explained in terms of nanotube curvature and atomic vibrations involving interaction among the walls in MWCNTs. The present study demonstrates the power of XRD for nondestructive evaluation of diameter distribution and interwall separation in MWCNTs with wide range of diameters.