Anomalous enhancement of magnetism by nonmagnetic doping in the honeycomb-lattice antiferromagnet ErOCl

TL;DR

This study demonstrates that nonmagnetic doping in ErOCl enhances magnetism through lattice distortion and increased magnetic anisotropy, revealing an unconventional mechanism contrary to typical magnetic dilution effects.

Contribution

It uncovers how chemical pressure from Lu^3+ doping enhances magnetic anisotropy and magnetization in ErOCl, challenging traditional views on magnetic dilution effects.

Findings

Magnetization per Er^3+ ion increases under high magnetic fields.

Lu^3+ doping causes c-axis contraction and increases CEF axial parameter B_2^0.

Enhanced magnetic anisotropy leads to higher low-temperature magnetization.

Abstract

Tuning magnetic anisotropy through chemical doping is a powerful strategy for designing functional materials with enhanced magnetic properties. Here, we report an enhanced Er^3+ magnetic moment resulting from nonmagnetic Lu^3+ substitution in the honeycomb-lattice antiferromagnet ErOCl. Unlike the Curie-Weiss type divergence typically observed in diluted magnetic systems, our findings reveal a distinct enhancement of magnetization per Er^3+ ion under high magnetic fields, suggesting an unconventional mechanism. Structural analysis reveals that Lu^3+ doping leads to a pronounced contraction of the c axis, which is attributed to chemical pressure effects, while preserving the layered SmSI-type crystal structure with space group R-3m. High-resolution Raman spectroscopy reveals a systematic blueshift of the first and seventh crystalline electric field (CEF) excitations, indicating an increase in the axial CEF parameter B_2^0. This modification enhances the magnetic anisotropy along the c axis, leading to a significant increase in magnetization at low temperatures and under high magnetic fields, contrary to conventional expectations for magnetic dilution. Our work not only clarifies the intimate connection between magnetism and CEF in rare-earth compounds, but more importantly, it reveals a physical pathway to effectively tune magnetic anisotropy via anisotropic lattice distortion induced by chemical pressure.