Achieving true bulk insulating behavior in Bi2Se3, the archetypal topological insulator with a simplistic one-band electronic structure and sizable band gap, has been prohibited by a well-known self-doping effect caused by selenium vacancies, whose extra electrons shift the chemical potential into the bulk conduction band. We report a new synthesis method for achieving stoichiometric Bi2Se3 crystals that exhibit nonmetallic behavior in electrical transport down to low temperatures. Hall effect measurements indicate the presence of both electron-and hole-like carriers, with the latter identified with surface state conduction and the achievement of ambipolar transport in bulk Bi2Se3 crystals without gating techniques. With carrier mobilities surpassing the highest values yet reported for topological surface states in this material, the achievement of ambipolar transport via upward band bending is found to provide a key method to advancing the potential of this material for future study and applications.
PACS numbers:The development of topological insulator (TI) materials has found rapid progress in the past few years [1]. Distinguished from ordinary insulators by the so-called Z 2 topological invariants associated with the bulk electronic band structure [2,3], this class of materials is characterized by nonlocal topology of the electronic structure that gives rise to new electronic states with promise for realizing new technologies such as fault-tolerant quantum computation [4]. By far the most widely studied system within the field of TI research is Bi 2 T 3 (T=Se,Te) [5][6][7][8][9][10]. To date, the major experimental efforts on these noninteracting bismuth-based TI materials have focused on refining measurement techniques in order to detect signatures of surface states. However, a continuing problem with the stoichiometric materials lies in the fact that they are not bulk insulators as predicted, but rather doped semiconductors [11]. Both bulk and surface quality of TI materials are known to dramatically affect their properties, with the effects of site exchange (e.g., in Bi 2 Te 3 ) or Se vacancy doping (e.g., in Bi 2 Se 3 ) serving to introduce excess charge carriers in the bulk (n-type with Bi 2 Se 3 and p-type with Bi 2 Te 3 ), reduce surface carrier mobilities and mix bulk and surface state conduction contributions.The common method of crystal growth using excess selenium falls short of reaching even a non-metallic temperature dependence of resistivity [12], which has to date produced samples with some of the lowest bulk carrier concentrations ever reported. Extensive work has been carried out to suppress bulk conductivity contributions by compensation doping [7,8,[13][14][15] but this has only been achieved in the binary materials by introducing excess impurity scattering via chemical substitution methods [16,17], such as was accomplished using Se-Te site substitution in the case of the ternary compound Bi 2 Te 2 Se [18,19]. Synthesis of defect-free epitaxial thin films [20,21] has also succeeded in redu...