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Part of Special Issue: Oxide superconductors and beyond - In memoriam of Professor Karl Alex Müller, Abstract: Discovery of high-Tc cuprate superconductors (HTSC) in 1986 by Bednorz and Muller, followed by synthesis of A3C60, iron-pnictides/chalcogenides and other exotic superconducting (SC) systems, introduced unconventional superconductors (UCSC) having their mechanisms of condensation and/or pairing distinctly different from those of simpler metals which can be explained by BCS theory. This article will show how one can demonstrate their new mechanisms by examining correlations among key energy-scale parameters, including the transition temperature Tc, the superfluid density ns/m*, the effective Fermi energy εF, the excitation energy of the magnetic resonance mode (MRM), the onset temperatures of Nernst effect and light-induced transient superconductivity, and the spin fluctuation energy scale ℏωsf, and by resorting to analogy / comparisons with superfluid 4He as a representative system undergoing Bose Einstein Condensation (BEC). We will propose a paring mechanism in HTSC based on resonance of spin (ℏωsf) and charge (εF) energy scales, and apply that concept for explaining unusual behaviors in the overdoped region. We will also discuss modifications of a simple BEC-BCS crossover picture to account for actual situations with additional effects of competing order and phase separation. 

Iron-chalcogenide superconductors FeSe_1−xS_xpossess 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 FeSe_1−xS_xsuperconductors for0≤x≤0.22covering both orthorhombic (nematic) and tetragonal phases. We find that the zero-field muon relaxation rate is enhanced below the superconducting transition temperatureT_cfor 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 FeSe_1−xS_x, which calls for the theory of microscopic origins that account for the relation between nematicity and superconductivity.