Termination-dependent topological surface states of the natural superlattice phase Bi4Se3

We describe the topological surface states of Bi4Se3, a compound in the infinitely adaptive Bi-2-Bi2Se3 natural superlattice phase series, determined by a combination of experimental and theoretical methods. Two observable cleavage surfaces, terminating at Bi or Se, are characterized by angle-resolved photoelectron spectroscopy and scanning tunneling microscopy, and modeled by ab initio density functional theory calculations. Topological surface states are observed on both surfaces, but with markedly different dispersions and Kramers point energies. Bi4Se3 therefore represents the only known compound with different topological states on differently terminated, easily distinguished and stable surfaces.