Honeycomb bismuthene structures on Ag(111) were investigated using low-energy electron diffraction (LEED) and density functional theory. LEED I(V) analysis revealed that 0.5 monolayer (ML) of Bi forms an ultraflat honeycomb lattice with negligible buckling at ∼120 K, which transforms into other structures upon warming to room temperature. A similar flat bismuthene structure also forms in Mn/Bi/Ag(111), which remains stable even at room temperature. Mn deposition on (p × $\sqrt{3}$)-rect Bi/Ag(111) induces Bi surface segregation, as confirmed by x-ray photoelectron spectroscopy, resulting in a p(2 × 2) honeycomb bismuthene. The detailed structural investigation provides fundamental basis for characterizing the two-dimensional topological properties of bismuthene grown on Ag(111).

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• Crystal structure
• Topological materials
• Surfaces
• First-principles calculations
• Low-energy electron diffraction
• X-ray photoelectron spectroscopy