Electrons and phonons in single layers of hexagonal indium chalcogenides from ab initio calculations

Abstract

We use density functional theory to calculate the electronic band structures, cohesive energies, phonon dispersions, and optical absorption spectra of two-dimensional In$_2$X$_2$ crystals, where X is S, Se, or Te. We identify two crystalline phases (alpha and beta) of monolayers of hexagonal In$_2$X$_2$, and show that they are characterized by different sets of Raman-active phonon modes. We find that these materials are indirect-band-gap semiconductors with a sombrero-shaped dispersion of holes near the valence-band edge. The latter feature results in a Lifshitz transition (a change in the Fermi-surface topology of hole-doped In$_2$X$_2$) at hole concentrations $n_{\rm S}=6.86\times 10^{13}$ cm$^{-2}$, $n_{\rm Se}=6.20\times 10^{13}$ cm$^{-2}$, and $n_{\rm Te}=2.86\times 10^{13}$ cm$^{-2}$ for X=S, Se, and Te, respectively, for alpha-In$_2$X$_2$ and $n_{\rm S}=8.32\times 10^{13}$ cm$^{-2}$, $n_{\rm Se}=6.00\times 10^{13}$ cm$^{-2}$, and $n_{\rm Te}=8.14\times 10^{13}$ cm$^{-2}$ for beta-In$_2$X$_2$.