First-principles predictions of the diversity in the atomic structures and electronic properties of the reconstructed Si(111)-7 × 7 surface

Abstract

The reconstructed Si(111)-7 × 7 surface is commonly described using the dimer-adatom-stacking-fault (DAS) model; however, its electronic properties and possible alternative reconstructions remain subjects of long-standing interest. Predicting diverse DAS-like reconstructions within such a large size remains highly challenging for conventional structure-search methods. Here, using a graph-theory-based structure prediction framework implemented in the RG² code, we systematically identify a series of low-energy reconstructions of the Si(111)-7 × 7 surface, including both stacking-fault DAS-type structures (DAS-d₈-T¹², DAS-d₈-T⁹H^3-A, DAS-d₈-T⁹H^3-B, and DAS-d₈-T⁶H⁶) and non-stacking-fault variants (AB-d₁₀-T¹², AB-d₁₀-T⁹H³, AA-d₁₀-T¹², and AA-d₁₀-T⁹H³). These reconstructions exhibit comparable energetic stability to the conventional DAS model and produce similar simulated STM contrasts, reflecting their close topological and electronic similarity. All identified reconstructions are metallic in the nonmagnetic state, characterized by isolated narrow surface bands near the Fermi level with different occupancies. Depending on band filling, they further exhibit a rich variety of electronic phases, including ferromagnetic metals, half-metals, half-semimetals, and insulators. In addition, electron and hole doping of the DAS structures can drive transitions into insulating phases, highlighting the sensitivity of the electronic properties to band occupancy. These results reveal the remarkable structural and electronic diversity of reconstructed Si(111)-7 × 7 surfaces and provide a unified framework for understanding how competing low-energy reconstructions and electronic filling effects can give rise to distinct electronic phases.