Stacking up electron-rich and electron-deficient monolayers to achieve extraordinary mid- to far-infrared excitonic absorption: Interlayer excitons in the C3B/C3N bilayer

TL;DR

This paper predicts that a heterostructure of C3N and C3B monolayers exhibits extraordinary mid- to far-infrared excitonic absorption due to interlayer excitons, using advanced many-body perturbation theory.

Contribution

It introduces a novel C3N/C3B heterostructure with strong interlayer excitonic effects in the infrared range, supported by first-principles calculations.

Findings

Supports bright interlayer excitons with large binding energies (0.2-0.4 eV).

Enables mid- to far-infrared applications at room temperature.

Reveals formation mechanisms of inter- and intra-layer excitons.

Abstract

Our ability to efficiently detect and generate far-infrared (i.e., terahertz) radiation is vital in areas spanning from biomedical imaging to interstellar spectroscopy. Despite decades of intense research, bridging the terahertz gap between electronics and optics remains a major challenge due to the lack of robust materials that can efficiently operate in this frequency range, and two-dimensional (2D) type-II heterostructures may be ideal candidates to fill this gap. Herein, using highly accurate many-body perturbation theory within the GW plus Bethe-Salpeter equation approach, we predict that a type-II heterostructure consisting of an electron rich C3N and an electron deficient C3B monolayers can give rise to extraordinary optical activities in the mid- to far-infrared range. C3N and C3B are two graphene-derived 2D materials that have attracted increasing research attention. Although both C3N and C3B monolayers are moderate gap 2D materials, and they only couple through the rather weak van der Waals interactions, the bilayer heterostructure surprisingly supports extremely bright, low-energy interlayer excitons with large binding energies of 0.2 ~ 0.4 eV, offering an ideal material with interlayer excitonic states for mid-to far-infrared applications at room temperature. We also investigate in detail the properties and formation mechanism of the inter- and intra-layer excitons.