Magnetic anisotropy and dipolar interactions in the frustrated triangular-lattice magnet NaGdS_2

TL;DR

This study investigates the magnetic properties of NaGdS_2, revealing weak antiferromagnetic exchange, absence of long-range order, and the influence of dipolar interactions leading to short-range ferromagnetic correlations.

Contribution

It provides a comprehensive experimental and simulation analysis of NaGdS_2, highlighting the role of dipolar interactions in suppressing magnetic order in a Gd-based triangular-lattice magnet.

Findings

NaGdS_2 has weak antiferromagnetic exchange (~52mK).

Short-range magnetic order appears below 180 mK.

Dipolar interactions significantly influence magnetic behavior.

Abstract

In this comprehensive study, we present results of bulk measurements (magnetization, specific heat, ac susceptibility, thermal expansion, and magnetostriction) combined with local methods such as nuclear magnetic resonance (^23Na NMR) and electron spin resonance (ESR) and simulations (McPhase) on polycrystalline and single-crystalline NaGdS_2 samples. The rare-earth delafossite NaGdS_2 is a triangular-lattice magnet with S = 7/2 spin-only Gd^3+ moments with suppressed single-ion anisotropy. In our study, we estimate that NaGdS_2 has a weak antiferromagnetic exchange (J_H/k_B is about 52mK) and signs of long-range magnetic order are absent down to lowest temperature. However, indications of short range magnetic order are found below 180 mK in the ac susceptibility and thermal expansion. Our results indicate an interplay of Heisenberg-type and dipolar exchange. Due to the large moment of the Gd^3+ ions, one expects a strong impact of the dipolar coupling in NaGdS_2, in contrast to the related NaYbS_2. ESR and ^23Na NMR measurements, indeed, indicate the formation of short-range ferromagnetic correlations. NaGdS_2 appears to be a rare system, in which magnetic order is suppressed by a competition between Heisenberg and dipolar interactions.