Multipolar fluctuations from localized 4f electrons in CeRh2As2

TL;DR

This study investigates the multipolar fluctuations in CeRh2As2, revealing dominant magnetic and electric multipole interactions among localized 4f electrons that influence its phase transitions and magnetic properties.

Contribution

The paper provides a detailed theoretical analysis of multipolar susceptibilities and interactions in CeRh2As2 using advanced computational methods, clarifying the nature of its order parameters.

Findings

Magnetic fluctuations are dominated by q=(1/2,1/2,0) within the CEF ground-state doublet.

Leading magnetic octupole fluctuations of z(x^2-y^2) symmetry are identified.

Electric quadrupole fluctuations of x^2-y^2 and {yz, zx} symmetries are significant.

Abstract

The heavy-fermion superconductor CeRh2As2 exhibits a non-superconducting phase transition that precedes the emergence of superconductivity. The nature of the corresponding order parameter remains under debate, with competing proposals involving magnetic dipoles or electric quadrupoles. We derive the momentum-dependent multipolar susceptibilities and effective interactions among the localized 4f electrons, based on the framework of density functional theory combined with dynamical mean-field theory. Magnetic fluctuations within the crystalline-electric-field (CEF) ground-state doublet are dominated by q=(1/2,1/2,0), corresponding to a two-dimensional checkerboard configuration of the magnetic moment M_z along the c axis. Hybridization between the CEF ground-state and the first-excited doublet gives rise to leading magnetic octupole fluctuations of z(x^2-y^2) symmetry, followed by electric quadrupole fluctuations of x^2-y^2 and {yz, zx} symmetries. By taking into account the anisotropic magnetic-field dependence of the transition temperature T_0, we conclude that an antiferromagnetic order of M_z at q=(1/2,1/2,0) is consistent with the experiments, owing to the enhancement of T_0 caused by fluctuations of the field-induced quadrupole of {yz, zx} type under an in-plane magnetic field.