Two superconducting states with broken time-reversal symmetry in FeSe1-xSx.

Iron-chalcogenide superconductors FeSe1-xSx possess 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-xSx superconductors for 0 ≤ x ≤ 0.22 covering both orthorhombic (nematic) and tetragonal phases. We find that the zero-field muon relaxation rate is enhanced below the superconducting transition temperature Tc for all compositions, indicating that the superconducting state breaks TRS both in the nematic and tetragonal phases. Moreover, the transverse-field µSR 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.

Nematic quantum critical point without magnetism in FeSe1-xSx superconductors.

In most unconventional superconductors, the importance of antiferromagnetic fluctuations is widely acknowledged. In addition, cuprate and iron-pnictide high-temperature superconductors often exhibit unidirectional (nematic) electronic correlations, including stripe and orbital orders, whose fluctuations may also play a key role for electron pairing. In these materials, however, such nematic correlations are intertwined with antiferromagnetic or charge orders, preventing the identification of the essential role of nematic fluctuations. This calls for new materials having only nematicity without competing or coexisting orders. Here we report systematic elastoresistance measurements in FeSe1-xSx superconductors, which, unlike other iron-based families, exhibit an electronic nematic order without accompanying antiferromagnetic order. We find that the nematic transition temperature decreases with sulfur content x; whereas, the nematic fluctuations are strongly enhanced. Near [Formula: see text], the nematic susceptibility diverges toward absolute zero, revealing a nematic quantum critical point. The obtained phase diagram for the nematic and superconducting states highlights FeSe1-xSx as a unique nonmagnetic system suitable for studying the impact of nematicity on superconductivity.