Versatile Method of Engineering the Band Alignment and the Electron Wavefunction Hybridization of Hybrid Quantum Devices

Hybrid devices that combine superconductors (S) and semiconductors (Sm) have attracted great attention due to the integration of the properties of both materials, which relies on the interface details and the resulting coupling strength and wavefunction hybridization. However, until now, none of the experiments have reported good control of the band alignment of the interface, as well as its tunability to the coupling and hybridization. Here, the interface is modified by inducing specific argon milling while maintaining its high quality, e.g., atomic connection, which results in a large induced superconducting gap and ballistic transport. By comparing with Schrödinger–Poisson calculations, it is proven that this method can vary the band bending/coupling strength and the electronic spatial distribution. In the strong coupling regime, the coexistence and tunability of crossed Andreev reflection and elastic co‐tunneling—key ingredients for the Kitaev chain—are confirmed. This method is also generic for other materials and achieves a hard and huge superconducting gap in lead and indium antimonide nanowire (Pb‐InSb) devices. Such a versatile method, compatible with the standard fabrication process and accompanied by the well‐controlled modification of the interface, will definitely boost the creation of more sophisticated hybrid devices for exploring physics in solid‐state systems. The versatile approach is fully compatible with the lithography processes to create an atomically connected interface and effectively modulate the band alignment at the interface. This method is also generic for other materials and will ultimately result in the desirable requirements for topological and Andreev devices.