Semiconductor–superconductor hybrids are widely used to realize complex quantum phenomena, such as topological superconductivity and spins coupled to Cooper pairs. Accessing new, exotic regimes at high magnetic fields and increasing operating temperatures beyond the state-of-the-art requires new, epitaxially matched semiconductor–superconductor materials. One challenge is the generation of favourable conditions for heterostructural formation between materials with the desired properties. Here we harness an increased knowledge of metal-on-semiconductor growth to develop InAs nanowires with epitaxially matched, single-crystal, atomically flat Pb films with no axial grain boundaries. These highly ordered heterostructures have a critical temperature of 7 K and a superconducting gap of 1.25 meV, which remains hard at 8.5 T, and therefore they offer a parameter space more than twice as large as those of alternative semiconductor–superconductor hybrids. Additionally, InAs/Pb island devices exhibit magnetic field-driven transitions from a Cooper pair to single-electron charging, a prerequisite for use in topological quantum computation. Semiconductor–Pb hybrids potentially enable access to entirely new regimes for a number of different quantum systems.

Little–Parks oscillations of a hollow superconducting cylinder are of interest for flux-driven topological superconductivity in single Rashba nanowires. The oscillations are typically symmetric in the orientation of the applied magnetic flux. Using double InAs nanowires coated by an epitaxial superconducting Al shell which, despite the non-centro-symmetric geometry, behaves effectively as one hollow cylinder, we demonstrate that a small misalignment of the applied parallel field with respect to the axis of the nanowires can produce field-asymmetric Little–Parks oscillations. These are revealed by the simultaneous application of a magnetic field perpendicular to the misaligned parallel field direction. The asymmetry occurs in both the destructive regime, in which superconductivity is destroyed for half-integer quanta of flux through the shell, and in the non-destructive regime, where superconductivity is depressed but not fully destroyed at these flux values.