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arXiv · 2203.16295

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

Victor Porée·Elsa Lhotel·Sylvain Petit·Aleksandra Krajewska·Pascal Puphal·Adam H. Clark·Vladimir Pomjakushin·Helen C. Walker·Nicolas Gauthier·Dariusz J. Gawryluk·Romain Sibille
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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$_7$.

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Victor Porée, Elsa Lhotel, Sylvain Petit, Aleksandra Krajewska, Pascal Puphal, Adam H. Clark, Vladimir Pomjakushin, Helen C. Walker, Nicolas Gauthier, Dariusz J. Gawryluk, Romain Sibille. 2022-03-30. Crystal-field states and defect levels in candidate quantum spin ice Ce$_{2}$Hf$_{2}$O$_{7}$. https://doi.org/10.1103/physrevmaterials.6.044406

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