Unconventional bright ground-state excitons in monolayer TiI2 from first-principles calculations

Abstract Based on ab initio screened configuration interaction calculations we find that TiI 2 has a bright exciton ground state and identify two key mechanisms that lead to this unprecedented feature among transition metal dichalcogenides. First, the spin-orbit induced conduction band splitting results in optically allowed spin-alignment for electrons and holes across a significant portion of the Brillouin zone around the K -valley, avoiding band crossings seen in materials like monolayer MoSe 2 . Second, a sufficiently weak exchange interaction ensures that the bright exciton remains energetically below the dark exciton state. We further show that the bright exciton ground state is stable under various mechanical strains and that trion states (charged excitons) inherit this bright ground state. Our findings are expected to spark further investigation into related materials that bring along the two key features mentioned, as bright ground-state excitons are crucial for applications requiring fast radiative recombination.