Atomistic Compositional Details and Their Importance for Spin Qubits in Isotope‐Purified Silicon Quantum Wells

Abstract Understanding crystal characteristics down to the atomistic level increasingly emerges as a crucial insight for creating solid state platforms for qubits with reproducible and homogeneous properties. Here, isotope concentration depth profiles in a SiGe/²⁸Si/SiGe heterostructure are analyzed with atom probe tomography (APT) and time‐of‐flight secondary‐ion mass spectrometry down to their respective limits of isotope concentrations and depth resolution. Spin‐echo dephasing times and valley energy splittings E_VS around have been observed for single spin qubits in this quantum well (QW) heterostructure, pointing toward the suppression of qubit decoherence through hyperfine interaction with crystal host nuclear spins or via scattering between valley states. The concentration of nuclear spin‐carrying ²⁹Si is 50 ± 20ppm in the ²⁸Si QW. The resolution limits of APT allow to uncover that both the SiGe/²⁸Si and the ²⁸Si/SiGe interfaces of the QW are shaped by epitaxial growth front segregation signatures on a few monolayer scale. A subsequent thermal treatment, representative of the thermal budget experienced by the heterostructure during qubit device processing, broadens the top SiGe/²⁸Si QW interface by about two monolayers, while the width of the bottom ²⁸Si/SiGe interface remains unchanged. Using a tight‐binding model including SiGe alloy disorder, these experimental results suggest that the combination of the slightly thermally broadened top interface and of a minimal Ge concentration of % in the QW, resulting from segregation, is instrumental for the observed large . Minimal Ge additions <1%, which get more likely in thin QWs, will hence support high E_VS without compromising coherence times. At the same time, taking thermal treatments during device processing as well as the occurrence of crystal growth characteristics into account seems important for the design of reproducible qubit properties.