Origin of layer number dependent linear and nonlinear optical properties of two-dimensional graphene-like SiC

TL;DR

This paper investigates the layer-dependent linear and nonlinear optical properties of 2D graphene-like SiC, revealing how layer number influences dielectric and second harmonic generation responses through detailed electronic transition analysis.

Contribution

It provides a theoretical explanation for the layer-dependent optical properties of 2D SiC, highlighting the role of interlayer and intraband transitions in these phenomena.

Findings

Peak intensities of dielectric and SHG coefficients depend on layer number.

Distinct transition peaks are identified for different polarizations and layer configurations.

Interlayer transitions contribute to unique spectral features in multilayer SiC.

Abstract

We theoretically discuss the physical origin of the dielectric constants [{\epsilon}({\omega})] and second harmonic generation coefficients [\{chi}(2)({\omega})] of the ABA-stacked two-dimensional graphene-like silicon carbide (2D-SiC) with the number of layers up to 5. It is found that the intensities of the pronounced peaks of both {\epsilon}({\omega}) and \{chi}(2)({\omega}) exhibit a clear layer number dependence. For the light polarization parallel to the 2DSiC plane, the monolayer SiC (ML-SiC) and multilayer SiC (MuL-SiC) have very similar pronounced peak positions of {\epsilon}({\omega}), which are attributed to the {\pi}->{\pi}* and {\sigma}->{\sigma}* transitions. However, for the light polarization perpendicular to the 2D-SiC plane, a characteristic peak is found for the MuL-SiC at about 4.0 eV, except that the allowed {\pi}->{\sigma}* and {\sigma}->{\pi}* transition peaks are found for both ML-SiC and MuL-SiC in the high-energy region (> 8 eV). This characteristic peak is attributed to the interlayer {\pi}->{\pi}* transition which does not exist for the ML-SiC, and at this peak position, the ML-SiC has a weak dark exciton based on the mBJ calculation within the Bethe-Salpeter equation framework. For \{chi}(2)({\omega}), the single-particle transition channels based on the three-band terms dominate the second harmonic generation process of both ML-SiC and MuL-SiC and determine the size and sign of \{chi}(2)({\omega}). In the ultraviolet visible region, the purely interband motion and intraband motion of electrons competitively determine the size and sign of \{chi}(2)({\omega}). For the light polarization perpendicular to the 2D-SiC plane, the intraband motion of electrons modulated more dramatically the interband motion than for that parallel to the 2D-SiC plane.