Evaluating the Effects of Structural Disorder on the Magnetic Properties of Nd${}_2$Zr${}_2$O${}_7$

Abstract

Motivated by the variation in reported lattice parameters of floating-zone-grown Nd${}_2$Zr${}_2$O${}_7$ crystals, we have performed a detailed study of the relationship between synthesis environment, structural disorder, and magnetic properties. Using a combination of polycrystalline standards, electron-probe microanalysis and scattering techniques, we show that crystals grown under atmospheric conditions have a reduced lattice parameter - relative to pristine polycrystalline powders - due to occupation of the Nd-site by excess Zr (i.e. "negative" stuffing). In contrast, crystals grown under high-pressure Ar are nearly stoichiometric with an average lattice parameter approaching the polycrystalline value. While minimal disorder of the oxygen sublattices is observed on the scale of the average structure, neutron pair-distribution function analysis indicates a highly local disorder of the oxygen coordination, which is only weakly dependent on growth environment. Most importantly, our magnetization, heat capacity and single-crystal neutron scattering data show that the magnetic properties of crystals grown under high-pressure Ar match closely with those of stoichiometric powders. Neutron scattering measurements reveal that the signature of magnetic moment fragmentation - the coexistence of all-in-all-out (AIAO) magnetic Bragg peaks and diffuse pinch-point scattering due to spin-ice correlations - persists in these nearly stoichiometric crystals. However, in addition to an increased AIAO transition temperature, the diffuse signal is seemingly stabilized and remains nearly unchanged upon warming to 800 mK. This behavior indicates that both the AIAO magnetic order and spin-ice correlations are sensitive to deviations of the Nd stoichiometry.

arXiv comment12 pages, 10 figures

References in corpus (28)

• Mantid - Data Analysis and Visualization Package for Neutron Scattering and $\mu SR$ Experiments
• Magnetic Pyrochlore Oxides
• The "Coulomb phase" in frustrated systems
• Disorder-Induced Mimicry of a Spin Liquid in YbMgGaO${}_4$
• Frustrated quantum rare-earth pyrochlores
• Experimental signatures of a three-dimensional quantum spin liquid in effective spin-1/2 Ce2Zr2O7 pyrochlore
• Quantum spin ices and topological phases from dipolar-octupolar doublets on the pyrochlore lattice
• Magnetic-Moment Fragmentation and Monopole Crystallization
• Lightly stuffed pyrochlore structure of single-crystalline Yb2Ti2O7 grown by the optical floating zone technique
• Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce${}_2$Zr${}_2$O${}_7$
• A quantum liquid of magnetic octupoles on the pyrochlore lattice
• Investigation of the magnetic structure and crystal field states of pyrochlore antiferromagnet Nd2Zr2O7
• Fluctuations and all-in$-$all-out ordering in dipole-octupole Nd2Zr2O7
• Vacancy defects and monopole dynamics in oxygen-deficient pyrochlores
• Symmetry Enriched U(1) Topological Orders for Dipole-Octupole Doublets on a Pyrochlore Lattice
• The quantum origins of moment fragmentation in Nd2Zr2O7
• Structural and Magnetic Investigations of Single-Crystals of the Neodymium Zirconate Pyrochlore, Nd2Zr2O7
• Pyrochlore U(1) spin liquid of mixed symmetry enrichments in magnetic fields
• Role of defects in determining the magnetic ground state of ytterbium titanate
• Order out of a Coulomb phase and Higgs transtion: frustrated transverse interactions of Nd2Zr2O7
• Dilute stuffing in the pyrochlore iridate $E{u}_{2}I{r}_2{O}_7$
• Dipolar-Octupolar Ising Antiferromagnetism in Sm${}_2$Ti${}_2$O${}_7$: A Moment Fragmentation Candidate
• Dynamic quantum kagome ice
• High-Pressure Laser Floating Zone Furnace
• Spin dynamics and unconventional Coulomb phase in Nd${}_2$Zr${}_2$O${}_7$
• Anisotropic exchange Hamiltonian, magnetic phase diagram and domain inversion of Nd${}_2$Zr${}_2$O${}_7$
• Evolution of antiferromagnetic domains in the all-in-all-out ordered pyrochlore Nd${}_2$Zr${}_2$O${}_7$
• The pyrochlore Ho2Ti2O7: Synthesis, crystal growth and stoichiometry

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• Advances in high-pressure laser floating zone growth: the Laser Optical Kristallmacher II
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