Second-Harmonic Current-Phase Relation in Josephson Junctions with Ferromagnetic Barriers.

We report the observation of a current-phase relation dominated by the second Josephson harmonic in superconductor-ferromagnet-superconductor junctions. The exotic current-phase relation is realized in the vicinity of a temperature-controlled 0-to-π junction transition, at which the first Josephson harmonic vanishes. Direct current-phase relation measurements, as well as Josephson interferometry, nonvanishing supercurrent and half-integer Shapiro steps at the 0-π transition self-consistently point to an intrinsic second harmonic term, making it possible to rule out common alternative origins of half-periodic behavior. While surprising for diffusive multimode junctions, the large second harmonic is in agreement with theory predictions for thin ferromagnetic interlayers.