Possible Quadrupole Density Wave in the Superconducting Kondo Lattice CeRh2As2

CeRh2As2 has recently been reported to be a rare case of a multiphase unconventional superconductor close to a quantum critical point (QCP). Here, we present a comprehensive study of its normal-state properties and of the phase (I) below T-0 approximate to 0.4 K which preempts superconductivity at T-c = 0.26 K. The second-order phase transition at T-0 presents signatures in specific heat and thermal expansion but none in magnetization and ac susceptibility, indicating a nonmagnetic origin of phase I. In addition, an upturn of the in-plane resistivity at T-0 points to a gap opening at the Fermi level in the basal plane. Thermal expansion indicates a strong-positive-pressure dependence of T-0, dT(0)/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 T-0 to higher temperatures and transforms phase I into another nonmagnetic phase (II) through a first-order phase transition at about 9 T. Using renonnalized band-structure calculations, we find that the Kondo effect (T-K approximate to 30 K) leads to substantial mixing of the excited crystalline-electric-field 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 causes an unprecedented case of phase transition into a quadrupole-density-wave state at a temperature T-0 << T-K, which explains the nature of phases I and II.