Atypical antiferromagnetic ordering in single crystalline quasi-2D honeycomb magnet YbI$_3$

TL;DR

This study characterizes YbI3, a quasi-2D honeycomb magnet, revealing its magnetic ordering, anisotropy, and potential unconventional ground state through crystal growth and various spectroscopic and magnetic measurements.

Contribution

First detailed synthesis and characterization of high-quality YbI3 single crystals, revealing its magnetic properties and potential unconventional magnetic ground state.

Findings

YbI3 exhibits short-range and long-range magnetic ordering at 0.95 K and 0.6 K.

Magnetic susceptibility indicates easy-plane anisotropy.

Heat capacity suggests an unconventional magnetic ground state.

Abstract

Here, we study YbI$_3$, a quasi-2D layered material with Yb atoms arranged on an ideal honeycomb network of edge-sharing YbI$_6$ octahedra, analogous to the low-temperature phase of $\alpha-$RuCl$_3$. High quality single crystals of YbI$_3$ are grown from Yb and I as starting precursors, using the vapor transport technique. The grown crystals are characterized by single crystal x-ray diffraction, Raman spectroscopy, magnetization, and heat capacity probes. The crystal-field split ground state of Yb$^{3+}$ in \Yb~ is a well-isolated Kramers doublet with an effective moment $\rm J_{eff} = 1/2$. Upon cooling, the low-temperature heat capacity of \Yb~ reveals a broad peak at $\rm T_1 = 0.95$~K due to short-range ordering of the Yb moments, followed by a sharp peak at $\rm T_2 = T_N = 0.6$~K due to long-range ordering. The magnetic behavior is found to be weakly anisotropic with $\chi^\parallel > \chi^\perp$, where $\chi^\parallel$ and $\chi^\perp$ refers to the in-plane ($H \parallel ab$) and out-of-plane ($H \perp ab$) susceptibilities. The 2~K isothermal magnetization saturates at $\rm \approx~1.5~\mu_B/Yb^{3+}$ (in-plane) and $\rm \approx~1~\mu_B/Yb^{3+}$ (out-of-plane), suggesting the anisotropy to be easy-plane type. Low-temperature heat capacity, well below T$_N$, is found to vary as T$^\alpha$ with $\alpha~\approx~2.5$, indicating a possible unconventional magnetic ground state for YbI$_3$.