Quadrupole partial orders and triple-$q$ states on the face-centered cubic lattice

Abstract

We study ${\Gamma }_3$ quadrupole orders in a face-centered cubic lattice. The ${\Gamma }_3$ quadrupole moments under cubic symmetry possess a unique cubic invariant in their free energy in the uniform ($q=0$) sector and the triple-q sector for the X points $q=(2\pi ,0,0),(0,2\pi ,0)$, and $(0,0,2\pi )$. Competition between this cubic anisotropy and anisotropic quadrupole-quadrupole interactions causes a drastic impact on the phase diagram both in the ground state and at finite temperatures. We show details about the model construction and its properties, the phase diagram, and the mechanism of the various triple-$q$ quadrupole orders reported in our preceding letter [J. Phys. Soc. Jpn. 90, 43701 (2021), arXiv:2102.06346]. By using a mean-field approach, we analyze a quadrupole exchange model that consists of a crystalline-electric field scheme with the ground-state ${\Gamma }_3$ non-Kramers doublet and the excited singlet ${\Gamma }_1$ state. We find various triple-$q$ orders in the four-sublattice mean-field approximation. A few partial orders of quadrupoles are stabilized in a wide range of parameter space at a higher transition temperature than single-$q$ orders. With lowering the temperature, these partial orders undergo phase transitions into further symmetry broken phases in which nonvanishing quadrupole moments emerge at previously disordered sites. The obtained phases in the mean-field approximation are investigated by a phenomenological Landau theory, which clearly shows that the cubic invariant plays an important role for stabilizing the triple-$q$ states. We also discuss its implications for recent experiments in a few f- and d-electron compounds.

28 pages, 20 figures

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