Optimized flux single-crystal growth of the quantum spin liquid candidate NdTa$_7$O$_{19}$ and other rare-earth heptatantalates, ErTa$_7$O$_{19}$ and GdTa$_7$O$_{19}$

TL;DR

This paper presents a flux method to grow large single crystals of NdTa$_7$O$_{19}$, a quantum spin liquid candidate, and explores the magnetic properties of NdTa$_7$O$_{19}$, ErTa$_7$O$_{19}$, and GdTa$_7$O$_{19}$, revealing significant anisotropy and potential exotic magnetic states.

Contribution

The study introduces a novel flux growth technique for large single crystals of NdTa$_7$O$_{19}$ and related compounds, enabling detailed magnetic characterization of these rare-earth heptatantalates.

Findings

NdTa$_7$O$_{19}$ crystals exhibit substantial magnetic anisotropy without long-range order down to 2 K.

ErTa$_7$O$_{19}$ shows similar anisotropic magnetic behavior to NdTa$_7$O$_{19}$, suggesting similar exotic states.

GdTa$_7$O$_{19}$ displays paramagnetic behavior consistent with previous polycrystalline results.

Abstract

Single crystals are essential for characterizing a wide range of magnetic states, including exotic ones such as quantum spin liquids. This study reports a flux method for growing single crystals of NdTa$_7$O$_{19}$, the first quantum spin liquid candidate on a triangular spin lattice with dominant Ising like spin correlations. Purple NdTa$_7$O$_{19}$ single crystals with hexagonal morphology were successfully grown using a K$_2$Mo$_3$O$_{10}$-B$_2$O$_3$ flux. With lateral sizes up to 3.5 mm and a thickness up to 2 mm, these are the largest dimensions reported to date. The chemical composition was confirmed by powder and single-crystal X-ray diffraction along with scanning electron microscopy with energy dispersive X-ray spectroscopy. Aiming for an accurate determination of the magnetic anisotropy and its effect on the magnetic properties, NdTa$_7$O$_{19}$ crystals were additionally analyzed by magnetic susceptibility, revealing a substantial anisotropy without long-range magnetic ordering down to 2 K. Single crystals of two novel rare-earth heptatantalates, ErTa$_7$O$_{19}$ and GdTa$_7$O$_{19}$, were also grown and their magnetic properties investigated. The magnetic anisotropy of ErTa$_7$O$_{19}$ closely resembles that of isostructural NdTa$_7$O$_{19}$, indicating a possibility of a similar exotic magnetic ground state. In contrast, GdTa$_7$O$_{19}$ shows paramagnetic behavior, consistent with previous results obtained for polycrystalline samples.