Giant Narrow-Band Optical Absorption and Distinctive Excitonic Structures of Monolayer and
Zhao Tang, Greis J. Cruz, Yabei Wu, Weiyi Xia, Fanhao Jia, Wenqing Zhang, and Peihong Zhang
Phys. Rev. Applied 17, 034068 (2022) - Published 28 March, 2022
Low-dimensional materials provide a unique platform for exploring exotic properties that are otherwise unachievable in bulk solids. and are two graphene-derived two-dimensional (2D) ordered alloys that have attracted increasing research attention. These materials are best known for their remarkable stability and moderate band gaps, and thus, are suitable for a range of applications. Perhaps the most interesting feature of the electronic structures of and is the existence of nearly parallel valence and conduction bands across a large region of the Brillouin zone. In this work, using many-body perturbation theory within the GW and Bethe–Salpeter-equation approach, we predict that the primarily -orbital-derived nearly parallel valence and conduction bands in monolayer and give rise to a giant narrow-band absorption peak in their optical absorption spectra. More surprisingly, two degenerate excitonic states contribute to over 90% and 80% of the dipole absorption below 5 eV for and , respectively. Detailed examinations of the exciton-binding energies unveil a unique shell-like distribution of the excitonic states, with each shell (series) converging to a different excitation edge. Such distinctive absorption properties are not observed in any other 2D materials. We further investigate the internal structure of the excitonic states using a multifaceted approach and reveal several important characteristics of the excitonic states in these 2D materials.


