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Termination-dependent surface properties in the giant-Rashba semiconductors BiTeX (X = Cl, Br, I)

The non-centrosymmetric semiconductors BiTeX (X = Cl, Br, I) show large Rashba-type spin-orbit splittings in their electronic structure making them candidate materials for spin-based electronics. However, BiTeI(0001) single crystal surfaces usually consist of stacking-fault-induced domains of Te and I terminations implying a spatially inhomogeneous electronic structure. Here we combine scanning tunneling microscopy (STM), photoelectron spectroscopy (ARPES, XPS) and density functional theory (DFT) calculations to systematically investigate the structural and electronic properties of BiTeX(0001) surfaces. For X = Cl, Br we observe macroscopic single-terminated surfaces. We discuss chemical characteristics among the three materials in terms of bonding character, surface electronic structure, and surface morphology.