Continuum excitation and pseudospin wave in quantum spin-liquid and quadrupole ordered states of Tb${}_{2+x}$Ti${}_{2-x}$O${}_{7+y}$

Abstract

The ground states of the frustrated pyrochlore oxide Tb${}_{2+x}$Ti${}_{2-x}$O${}_{7+y}$ have been studied by inelastic neutron scattering experiments. Three single-crystal samples are investigated; one shows no phase transition ($x=-0.007<x_{\text{c}}\sim -0.0025$), being a putative quantum spin-liquid (QSL), and the other two ($x=0.000,0.003$) show electric quadrupole ordering (QO) below $T_{\text{c}}\sim 0.5$ K. The QSL sample shows continuum excitation spectra with an energy scale 0.1 meV as well as energy-resolution limited (nominally) elastic scattering. As $x$ is increased, pseudospin wave of the QO state emerges from this continuum excitation, which agrees with that of powder samples and consequently verifies good $x$ control for the present single crystal samples.

arXiv comment7 pages, 4 figures

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• Spin correlations of quantum-spin-liquid and quadrupole-ordered states of Tb${}_{2+x}$Ti${}_{2-x}$O${}_{7+y}$
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• Traversing the pyrochlore stability diagram; microwave-assisted synthesis and discovery of mixed B-site Ln${}_2$InSbO${}_7$ family
• Spin and quadrupole correlations by three-spin interaction in the frustrated pyrochlore magnet Tb${}_{2+x}$Ti${}_{2-x}$O${}_{7+y}$
• Excitation spectrum and low-temperature magnetism in disordered defect-fluorite Ho2Zr2O7