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Intrinsic topological insulators  are realized by alloying Bi 2 Te 3  with Bi 2 Se 3 . Angle‐resolved photoemission and bulk transport measurements reveal that the Fermi level is readily tuned into the bulk bandgap. First‐principles calculations of the native defect landscape highlight the key role of anti‐site defects for achieving this, and predict optimal growth conditions to realize maximally resistive topological insulators.

Controlling Bulk Conductivity in Topological Insulators: Key Role of Anti‐Site Defects