Theoretical vibrational optical activity of chiral carbon nanoparticles: Fullerenes and carbon nanotubes

Abstract

A theoretical study of the first‐order resonance Raman optical activity (ROA) of a single‐walled carbon nanotube (SWCNT) is presented for the first time. Tight‐binding (TB) Raman and ROA scattering tensors are combined with precise first principles harmonic vibrational modes to obtain scattering intensities. This computational protocol for Raman and ROA spectra has been tested previously for chiral fullerenes, such as C [Nagy et al., J. Chem. Phys. 140, 044112 (2014)]. In the present study, this methodology is validated against density functional theory for the alternative case of C. TB spectral shapes are found to be reliable to determine the absolute configuration of these cage like carbon structures with relatively small curvature. Utilizing the same method, Raman optical activity (ROA) intensities of the (6,5) SWCNT are calculated for three vibrational modes, radial breathing mode (RBM), G, and G. This tube exhibits approximately 5 orders of magnitude stronger ROA intensity compared to typical chiral molecules.