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  1. 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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    Free, publicly-accessible full text available May 23, 2024
  2. null (Ed.)
    We use polarization-resolved electronic Raman spectroscopy to study quadrupolar charge dynamics in a nonmagnetic F e S e 1 − x S x superconductor. We observe two types of long-wavelength X Y symmetry excitations: 1) a low-energy quasi-elastic scattering peak (QEP) and 2) a broad electronic continuum with a maximum at 55 meV. Below the tetragonal-to-orthorhombic structural transition at T S ( x ) , a pseudogap suppression with temperature dependence reminiscent of the nematic order parameter develops in the X Y symmetry spectra of the electronic excitation continuum. The QEP exhibits critical enhancement upon cooling toward T S ( x ) . The intensity of the QEP grows with increasing sulfur concentration x and maximizes near critical concentration x c r ≈ 0.16 , while the pseudogap size decreases with the suppression of T S ( x ) . We interpret the development of the pseudogap in the quadrupole scattering channel as a manifestation of transition from the non-Fermi liquid regime, dominated by strong Pomeranchuk-like fluctuations giving rise to intense electronic continuum of excitations in the fourfold symmetric high-temperature phase, to the Fermi liquid regime in the broken-symmetry nematic phase where the quadrupole fluctuations are suppressed. 
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