Crystal-field states and defect levels in candidate quantum spin ice Ce$_{2}$Hf$_{2}$O$_{7}$

TL;DR

This study synthesizes and characterizes Ce$_{2}$Hf$_{2}$O$_{7}$, revealing its potential as a quantum spin ice candidate with unique magnetic and crystal-field properties, including a dipole-octupole ground state and absence of magnetic order down to very low temperatures.

Contribution

It provides detailed experimental analysis of Ce$_{2}$Hf$_{2}$O$_{7}$'s crystal-field states and defect levels, establishing its suitability for exploring exotic quantum magnetic states.

Findings

Ce$_{2}$Hf$_{2}$O$_{7}$ has a dipole-octupole ground state doublet.

No magnetic long-range order observed down to 0.08 K.

Significant spin-lattice coupling detected.

Abstract

We report the synthesis of powder and single-crystal samples of the cerium pyrohafnate and their characterization using neutron diffraction, thermogravimetry and X-ray absorption spectroscopy. We evaluate the amount of non-magnetic Ce$^{4+}$ defects and use this result to interpret the spectrum of crystal-electric field transitions observed using inelastic neutron scattering. The analysis of these single-ion transitions indicates the dipole-octupole nature of the ground state doublet and a significant degree of spin-lattice coupling. The single-ion properties calculated from the crystal-electric field parameters obtained spectroscopically are in good agreement with bulk magnetic susceptibility data down to about 1 K. Below this temperature, the behavior of the magnetic susceptibility indicates a correlated regime without showing any sign of magnetic long-range order or freezing down to 0.08 K. We conclude that Ce$_2$Hf$_2$O$_{7}$ is another candidate to investigate exotic correlated states of quantum matter such as the octupolar quantum spin ice recently argued to exist in the isostructural compounds Ce$_2$Sn$_2$O$_7$ and Ce$_2$Zr$_2$O$_7$.