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Possible quadrupole density wave in the superconducting Kondo lattice CeRh2As2

CeRh2As2 has recently been reported to be a rare case of multi-phase unconventional superconductor [S. Khim et al., arXiv:2101.09522] close to a quantum critical point (QCP). Here, we present a comprehensive study of its normal state properties and of the phase (I) below To ~ 0.4 K which preempts superconductivity at Tc = 0.26 K. The 2nd-order phase transition at To presents signatures in specific heat and thermal expansion, but none in magnetization and ac-susceptibility, indicating a non-magnetic origin of phase I. In addition, an upturn of the in-plane resistivity at To points to a gap opening at the Fermi level in the basal plane. Thermal expansion indicates a strong positive pressure dependence of To , dTo/dp = 1.5 K/GPa, in contrast to the strong negative pressure coefficient observed for magnetic order in Ce-based Kondo lattices close to a QCP. Similarly, an in-plane magnetic field shifts To to higher temperatures and transforms phase I into another non-magnetic phase (II) through a 1st-order phase transition at about 9 T. Using renormalized band structure calculations, we found that the Kondo effect (TK ~ 30 K) leads to substantial mixing of the excited crystalline-electric-field (CEF) states into the ground state. This allows quadrupolar degrees of freedom in the resulting heavy bands at the Fermi level which are prone to nesting. The huge sensitivity of the quadrupole moment on hybridization together with nesting would cause an unprecedented case of phase transition into a quadrupole-density-wave (QDW) state at a temperature To << TK , which would explain the nature of phase I and II.