We have investigated several strong spin-orbit coupling ternary chalcogenides related to the (Pb,Sn)Te series of compounds. Our first-principles calculations predict the low temperature rhombohedral ordered phase in TlBiTe2, TlBiSe2, and TlSbX2 (X=Te, Se, S) to be topologically Z2 = -1 nontrivial. We identify the specific surface termination that realizes the single Dirac cone through first-principles surface state computations. This termination minimizes effects of dangling bonds making it favorable for photoemission (ARPES) experiments. Our analysis predicts that thin films of these materials would harbor novel 2D quantum spin Hall states, and support odd-parity topological superconductivity. For a related work also see arXiv:1003.2615v1. Experimental ARPES results will be published elsewhere.
PACS numbers:Topological insulators are a recently discovered new phase of quantum matter [1][2][3]. The search for topological insulators in real materials has benefitted from the fruitful interplay between topological band theory of Kane and Mele (2005) and realistic band structure calculations [4][5][6][7][8][9][10][11][12]. As a result, Bi x Sb 1−x , Bi 2 Se 3 and Bi 2 Te 3 have been experimentally realized as three-dimensional topological insulators [6-9, 11, 12]. Recently, this search has been extended to ternary compounds [13,14]. Here, we report first-principles band calculations of Tl-based III-V-VI 2 ternary chalcogenide series, and compare the results to those of the related (Pb,Sn)Te series studied previously in connection with Dirac fermion physics in the 1980s [15]. The low temperature rhombohedral ordered phase in TlBiTe 2 , TlBiSe 2 , and TlSbX 2 (X=Te, Se, S) is predicted to be topologically nontrivial. Moreover, we have carried out first-principles slab computations in order to identify the specific surface termination which gives rise to the simple Dirac-cone surface band for ARPES measurements. An analysis of the symmetry of states indicates that thin films of the present materials would support 2D-quantum spin Hall states.Designing new topological insulators involves modifying atomic structure or doping to shift band orders out of the natural sequence. Consider, for example, the wellknown case of (Pb,Sn)Te with rocksalt structure. The end phase PbTe with face-centered cubic (FCC) lattice is topologically trivial. In contrast, SnTe has band inversions at four equivalent L-points where parities of conduction and valence bands are switched (Fig. 2E). Since this inversion occurs at an even number of points in the Brillouin zone, SnTe is also a topologically trivial band insulator. Fu and Kane [5] proposed that a rhombohedral distortion along a particular 111 direction can induce (Pb,Sn)Te into a strong topological phase because then the band inversion occurs only at the L-point along the 111 direction which is distinguished from the other three L-points (Fig. 1B).The Tl-based III-V-VI 2 ternary chalcogenides M M ′ X 2 are, or can be, approximately viewed as a rhombohedral structure with space group R3m[...