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Title: Two superconducting states with broken time-reversal symmetry in FeSe 1−x S x

Iron-chalcogenide superconductors FeSe1−xSxpossess unique electronic properties such as nonmagnetic nematic order and its quantum critical point. The nature of superconductivity with such nematicity is important for understanding the mechanism of unconventional superconductivity. A recent theory suggested the possible emergence of a fundamentally new class of superconductivity with the so-called Bogoliubov Fermi surfaces (BFSs) in this system. However, such an ultranodal pair state requires broken time-reversal symmetry (TRS) in the superconducting state, which has not been observed experimentally. Here, we report muon spin relaxation (μSR) measurements in FeSe1−xSxsuperconductors for0x0.22covering both orthorhombic (nematic) and tetragonal phases. We find that the zero-field muon relaxation rate is enhanced below the superconducting transition temperatureTcfor all compositions, indicating that the superconducting state breaks TRS both in the nematic and tetragonal phases. Moreover, the transverse-fieldμSR measurements reveal that the superfluid density shows an unexpected and substantial reduction in the tetragonal phase (x>0.17). This implies that a significant fraction of electrons remain unpaired in the zero-temperature limit, which cannot be explained by the known unconventional superconducting states with point or line nodes. The TRS breaking and the suppressed superfluid density in the tetragonal phase, together with the reported enhanced zero-energy excitations, are consistent with the ultranodal pair state with BFSs. The present results reveal two different superconducting states with broken TRS separated by the nematic critical point in FeSe1−xSx, which calls for the theory of microscopic origins that account for the relation between nematicity and superconductivity.

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Publisher / Repository:
National Academy of Sciences
Date Published:
Journal Name:
Proceedings of the National Academy of Sciences
Subject(s) / Keyword(s):
["iron-based superconductors","superconducting gap","muon spin relaxation","unconventional superconductivity","Bogoliubov Fermi surface"]
Medium: X
Sponsoring Org:
National Science Foundation
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