Multiple-excitation study of the double-resonance Raman bands in rhombohedral graphite

TL;DR

This study investigates the double-resonance Raman bands in rhombohedral graphite across multiple laser energies, revealing a richer and broader spectrum compared to Bernal graphite due to its larger Brillouin zone volume.

Contribution

It provides the first detailed dispersion analysis of DR Raman features in rhombohedral graphite using multiple excitation energies, highlighting its more complex spectral features.

Findings

Rhombohedral graphite exhibits broader, multi-peak 2D bands with distinct dispersive behaviors.

The larger Brillouin zone volume allows more resonance channels, enriching the Raman spectrum.

Spectral features in the 1700-1850 cm-1 range show complex intravalley phonon processes.

Abstract

The double-resonance (DR) Raman process is a signature of all sp2 carbon material and provide fundamental information of the electronic structure and phonon dispersion in graphene, carbon nanotubes and different graphite-type materials. We have performed in this work the study of different DR Raman bands of rhombohedral graphite using five different excitation laser energies and obtained the dispersion of the different DR features by changing the laser energy. Results are compared with those of Bernal graphite and shows that rhombohedral graphite exhibit a richer DR Raman spectrum. For example, the 2D band of rhombohedral graphite is broader and composed by several maxima that exhibit different dispersive behavior. The occurrence of more DR conditions in rhombohedral graphite is ascribed to the fact that the volume of its Brillouin zone (BZ) is twice the volume of the Bernal BZ, allowing thus more channels for the resonance condition. The spectra of the intervalley TO-LA band of rhombohedral graphite, around 2450 cm-1, is also broader and richer in features compared to that of Bernal graphite. Results and analysis of the spectral region 1700-1850 cm-1, where different intravalley processes involving acoustic and optical phonons occurs, are also presented.