AbstractProximity‐induced superconductivity in hybrid devices of topological insulators and superconductors offers a promising platform for the pursuit of elusive topological superconductivity and its anticipated applications, such as fault‐tolerant quantum computing. To study and harness such hybrid devices, a key challenge is the realization of highly functional material interfaces with a suitable superconductor featuring 2‐periodic parity‐conserving transport to ensure a superconducting hard‐gap free of unpaired electrons, which is important for Majorana physics. A superconductor well‐known for this characteristic is Al, however, its direct integration into devices based on tetradymite topological insulators has so far been found to yield non‐transparent interfaces. By focusing on Bi2Te3‐Al heterostructures, this study identifies detrimental interdiffusion processes at the interface through atomically resolved structural and chemical analysis, and showcases their mitigation by leveraging different interlayers – namely Nb, Ti, Pd, and Pt – between Bi2Te3 and Al. Through structural transformation of the interlayer materials (X) into their respective tellurides (XTe2) atomically‐sharp epitaxial interfaces are engineered and further characterized in low‐temperature transport experiments on Al‐X‐Bi2Te3‐X‐Al Josephson junctions and in complementary density functional theory calculations. By demonstrating functional interfaces between Bi2Te3 and Al, this work provides key insights and paves the way for the next generation of sophisticated topological devices.
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