Edge and Point-Defect Induced Electronic and Magnetic Properties in Monolayer PtSe2

Edges and point defects in layered dichalcogenides are important for tuning their electronic and magnetic properties. By combining scanning tunneling microscopy (STM) with density functional theory (DFT), the electronic structure of edges and point defects in 2D-PtSe2 are investigated where the 1.8 eV bandgap of monolayer PtSe2 facilitates the detailed characterization of defect-induced gap states by STM. The stoichiometric zigzag edge terminations are found to be energetically favored. STM and DFT show that these edges exhibit metallic 1D states with spin polarized bands. Various native point defects in PtSe2 are also characterized by STM. A comparison of the experiment with simulated images enables identification of Se-vacancies, Pt-vacancies, and Se-antisites as the dominant defects in PtSe2. In contrast to Se- or Pt-vacancies, the Se-antisites are almost devoid of gap states. Pt-vacancies exhibit defect induced states that are spin polarized, emphasizing their importance for inducing magnetism in PtSe2. The atomic-scale insights into defect-induced electronic states in monolayer PtSe2 provide the fundamental underpinning for defect engineering of PtSe2-monolayers and the newly identified spin-polarized edge states offer prospects for engineering magnetic properties in PtSe2 nanoribbons.

Automated summary

This study investigates the electronic structure of edges and point defects in 2D-PtSe2 using STM and DFT. The experiment finds that stoichiometric zigzag edge terminations are energetically favored, and Se-vacancies, Pt-vacancies, and Se-antisites are identified as dominant defects in PtSe2. Defects in PtSe2 are found to induce magnetism, with Pt-vacancies exhibiting spin polarized states. These atomic-scale insights into defect-induced electronic states provide fundamental support for defect engineering of PtSe2-monolayers and the potential for engineering magnetic properties in PtSe2 nanoribbons.