Evidence of pseudogap and absence of spin magnetism in the time-reversal-symmetry-breaking state of Ba_(1-x)K_xFe₂As₂

Muon-spin-rotation ($\mu$SR) experiments and the observation of a spontaneous Nernst effect indicate time-reversal symmetry breaking (BTRS) at $T_{\rm c}^{\rm Z2}$ above the superconducting transition temperature $T_{\rm c}$ in Ba$_{1-x}$K$_x$Fe$_2$As$_2$, with $x\approx0.8$. Further studies have pointed out that BTRS is caused by the formation of a new state of matter associated with the condensation of pairs of electron pairs. Despite exhibiting multiple unconventional effects that warrant further investigation, the electronic spectral properties of this electron quadrupling state remain largely unexplored. Here, we present detailed $^{75}$As nuclear magnetic resonance (NMR) measurements of Ba$_{1-x}$K$_x$Fe$_2$As$_2$, with $x = 0.77$, which has $T_{\rm c}^{\rm Z2}$ > $T_{\rm c}$ according to measurements of the spontaneous Nernst effect. The NMR data obtained in this work provide the first direct electronic spectral characteristics of the electron quadrupling state by indicating that it evolves from a pseudogap that sets in at $T^*$ well above $T_{\rm c}^{\rm Z2}$. This pseudogap behavior is consistent with $\mu$SR Knight-shift, specific-heat, and transport data indicating the formation of a bound state of electrons. According to a theory of electron quadrupling condensates, such bound-state formations should precede the onset of BTRS correlations between pairs of electron pairs. The second important insight from NMR data is the absence of spin-related magnetism. The temperature dependence of the spin-lattice relaxation rate $1/T_1T$ and the evolution of the NMR linewidth prove the absence of a magnetic transition at $T_{\rm c}^{\rm Z2}$ and rule out even a proximity to some magnetic instability. This indicates that the spontaneous magnetic fields detected in this compound are not caused by spin magnetism but are associated with persistent real-space currents.