Oxygen distribution and segregation at grain boundaries in Nb and Ta-encapsulated Nb thin films for superconducting qubits

We report on atomic-scale analyses of oxygen distribution and segregation at grain boundaries (GBs) of Nb and Ta-encapsulated Nb (Ta/Nb) thin films for superconducting qubits using atom-probe tomography (APT) and transmission electron microscopy (TEM). We observe oxygen segregation at grain boundaries (GBs) relative to the oxygen concentration within the grains for both Nb and Ta-capped Nb thin films for superconducting qubits and find that higher oxygen concentration in the interior of Nb grains lead to greater oxygen segregation levels at GBs. This finding emphasizes that controlling oxygen impurities in Nb during film deposition and fabrication processing is important to reduce the level of oxygen segregation at GBs in Nb. The enrichment factor (Cgb/Cgrain) for oxygen segregation at GBs in Nb is 2.7 (error bar: 0.3) for Nb films, and Ta-capped Nb thin films exhibit slightly reduced Nb GB enrichment factors of 2.3 (error bar: 0.3) while GBs in the Ta capping layer itself possess higher enrichment factors of 3.0 (error bar: 0.3). We hypothesize that the Ta capping layer can trap oxygen and thereby affect oxygen in-diffusion and segregation at GBs in the underlying Nb thin films. Finally, we find that increases in the oxygen concentration in both Nb grains and GBs correlate with a suppression in the critical temperature for superconductivity (Tc). Together, our comparative chemical and charge transport property analyses provide atomic-scale insights into a potential mechanism contributing to decoherence in superconducting qubits.