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Crystal-Field--Driven Magnetoelectricity in the Triangular Quantum Magnet CeMgAl₁1O₁9

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 ε'(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 ε'(T), exhibits a linear dependence on the squared magnetization M², 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.

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