Crystal-Field--Driven Magnetoelectricity in the Triangular Quantum Magnet CeMgAl$_{11}$O$_{19}$

Abstract

We report dielectric and magnetoelectric studies of single-crystalline \ce{CeMgAl11O19}, a Kramers triangular magnet embedded in a polarizable hexaaluminate lattice. In zero magnetic field, the permittivity $\varepsilon'(T)$ follows the Barrett law of a quantum paraelectric down to 25 K, below which a broad minimum develops near 3 K without evidence of static ferroelectric or magnetic order. Application of magnetic fields up to \SI{9}{\tesla} shifts this minimum to higher temperatures and broadens it, evidencing a tunable magnetoelectric response.The magnetoelectric coupling was characterized using results from magnetization measurements. The anomaly temperature $T^*$, extracted from the local minimum of $\varepsilon'(T)$, exhibits a linear dependence on the squared magnetization $M^2$, consistent with the biquadratic magnetoelectric coupling allowed in centrosymmetric systems. This magnetoelectric effect, mediated by spin-orbit-entangled Kramers doublets interacting with a frustrated antipolar liquid, establishes \ce{CeMgAl11O19} as a prototype for exploring quantum magnetoelectricity in frustrated systems.