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We successfully identified native point defects that occur in Bi2Te3 crystals by combining high-resolution bias-dependent scanning tunneling microscopy and density functional theory based calculations. As-grown Bi2Te3 crystals contain vacancies, antisites, and interstitial defects that may result in bulk conductivity and therefore may change the insulating bulk character. Here, we demonstrate the interplay between the growth conditions and the density of different types of native near-surface defects. In particular, scanning tunneling spectroscopy reveals the dependence on not only the local atomic environment but also on the growth kinetics and the resulting sample doping from n-type toward intrinsic crystals with the Fermi level positioned inside the energy gap. Our results establish a bias-dependent STM signature of the Bi2Te3 native defects and shed light on the link between the native defects and the electronic properties of Bi2Te3, which is relevant for the synthesis of topological insulator materials and the related functional properties.

We successfully identified native point defects that occur in Bi

Topological insulators (TIs) are renowned for their exotic topological surface states (TSSs) that reside in the top atomic layers, and hence, detailed knowledge of the surface top atomic layers is of utmost importance. Here we present the remarkable morphology changes of Bi2Te3 surfaces, which have been freshly cleaved in air, upon subsequent systematic annealing in ultrahigh vacuum and the resulting effects on the local and area-averaging electronic properties of the surface states, which are investigated by combining scanning tunneling microscopy (STM), scanning tunneling spectroscopy (STS), and Auger electron spectroscopy (AES) experiments with density functional theory (DFT) calculations. Our findings demonstrate that the annealing induces the formation of a Bi bilayer atop the Bi2Te3 surface. The adlayer results in n-type doping, and the atomic defects act as scattering centers of the TSS electrons. We also investigated the annealing-induced Bi bilayer surface on Bi2Te3 via voltage-dependent quasi-particle-interference (QPI) mapping of the surface local density of states and via comparison with the calculated constant-energy contours and QPI patterns. We observed closed hexagonal patterns in the Fourier transform of real-space QPI maps with secondary outer spikes. DFT calculations attribute these complex QPI patterns to the appearance of a second cone due to the surface charge transfer between the Bi bilayer and the Bi2Te3. Annealing in ultrahigh vacuum offers a facile route for tuning of the topological properties and may yield similar results for other topological materials.