Excitonic effects in the optical properties of SiC sheet and nanotubes

TL;DR

This study uses advanced ab initio methods to analyze excitonic effects and optical properties in SiC sheets and nanotubes, revealing significant quasiparticle corrections, exciton binding energies, and charge transfer characteristics.

Contribution

It provides the first detailed ab initio analysis of excitonic effects in SiC nanotubes and sheets, highlighting the impact of curvature and chirality on optical properties.

Findings

GW quasiparticle corrections exceed 1.0 eV

Exciton binding energies up to 2.0 eV observed

Charge transfer occurs from C to Si atoms in zigzag nanotubes

Abstract

The quasiparticle band structure and optical properties of single-walled zigzag and armchair SiC nanotubes (SiC-NTs) as well as single SiC sheet are investigated by ab initio many-body calculations using the GW and the GW plus Bethe-Salpeter equation (GW+BSE) approaches, respectively. Significant GW quasiparticle corrections of more than 1.0 eV to the Kohn-Sham band gaps from the local density approximation (LDA) calculations are found. The GW self-energy corrections transform the SiC sheet from a indirect LDA band gap to a direct band gap material. Furthermore, the quasiparticle band gaps of SiC-NTs with different chiralities behave very differently as a function of tube diameter, and this can be attributed to the difference in the curvature-induced orbital rehybridization between the different chiral nanotubes. The calculated optical absorption spectra are dominated by discrete exciton peaks due to exciton states with large binding energy up to 2.0 eV in the SiC sheet and SiC-NTs. The formation of strongly bound excitons is attributed to the enhanced electron-hole interaction in these low dimensional systems. Remarkably, the excited electron amplitude of the exciton wavefunction is found to peak on the Si atoms near the hole position (which is on the C site) in the zigzag SiC-NTs, indicating a charge transfer from an anion (hole) to its neighboring cations by photoexcitation. In contrast, this pronounced peak structure disappear in the exciton wavefunction in the armchair SiC-NTs. Furthermore, in the armchair SiC-NTs, the bound exciton wavefunctions are more localized and also strongly cylindrically asymmetric.