Thickness-modulated electronic band structures and exciton behavior of non-van-der-waals 2D Bi2O2Se films

Abstract

Bi2O2Se, as a non-van-der-waals (non-vdW) interlayer coupling two-dimensional material, its electronic band structures and exciton behavior still merit further in-depth studies, especially in the consideration of thickness tuning degrees of freedom. Here, we reveal the broadband excitonic performance and critical point properties of Bi2O2Se films with different thicknesses (3.54–16.33 nm). Five critical points are determined and assigned to specific optical transitions. Moreover, we observe that electronic bandstructures in the Γ valley are stable with variable thicknesses, while the deeper electron levels received more pronounced thickness modulation. And we first report four excitons in wide spectral range (1.24–6.20 eV) through absorption coefficient fitting. Significantly, due to the strong localization of electrons and holes induced by the intralayer built-in electric field, the exciton binding energy (Eb) value of 3.54 nm-Bi2O2Se (234 meV at Γ position) is apparently larger than typical multi-layer TMDCs, which offering unprecedented opportunities in applications in optoelectronic devices. Furthermore, Eb of two excitons at low energy region (Eb1, Eb2) red-shift with increasing thickness, while Eb of higher-energy excitons (Eb3, Eb4) blue-shift, owing to the dispersion characteristic of the effect dielectric screening effects. Our results are vital to wide-ranging applications of Bi2O2Se from fundamental science to optoelectronic devices.