Interfaces between materials with differently ordered phases present unique opportunities for exotic physical properties, especially the interplay between ferromagnetism and superconductivity in the ferromagnet/superconductor heterostructures. The investigation of zero- and pi-junctions has been of particular interest for both fundamental physical science and emerging technologies. Here, we report the experimental observation of giant oscillatory Gilbert damping in the superconducting Nb/NiFe/Nb junctions with respect to the NiFe thickness. This observation suggests an unconventional spin pumping and relaxation via zero-energy Andreev bound states that exist only in the Nb/NiFe/Nb pi-junctions, but not in the Nb/NiFe/Nb zero-junctions. Our findings could be important for further exploring the exotic physical properties of ferromagnet/superconductor heterostructures, and potential applications of ferromagnet pi-junctions in quantum computing, such as half quantum flux qubits.
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