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${}_{19}$

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.

24 pages, 11 figures, supplementary material