Structural Reconstruction Modulated Physical Properties of Titanium Oxide at the Monolayer Limit

To suppress surface dangling bonds, monolayer oxides derived from non-layered bulks usually undergo a pronounced structural reconstruction. It remains challenging to resolve these structural reconstructions and the induced distinct modulation of intrinsic properties. In this study, the structural reconstruction-modulated electronic, polaronic, and exitonic properties of a non-layered oxide at the monolayer limit are unraveled. Based on first-principles calculations and tight-binding simulations for a stable titanium dioxide (TiO2) monolayer, we show that its distinct surface Kagome sublattices host a topologically nontrivial flat band at the valence band edge. The strong electron–hole interaction in this monolayer oxide gives rise to a large exciton binding energy of around 2.49 eV. Interestingly, the monolayer TiO2 also exhibits strong electron–lattice coupling, which favors the formation of small electron polarons and thus greatly reduces its band gap energy into the visible light range. This work could be useful to understand the structural reconstruction-induced modulation of exotic physical and chemical properties for a broad range of non-layered oxides at the monolayer limit.