(2016) Antiferroquadrupolar correlations in the quantum spin ice candidate Pr2Zr2O7. Physical Review B, 94 (16). 165153 Permanent WRAP URL: http://wrap.warwick.ac.uk/87826
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Publisher statement: © 2016 American Physical Society
A note on versions:The version presented here may differ from the published version or, version of record, if you wish to cite this item you are advised to consult the publisher's version. Please see the 'permanent WRAP URL' above for details on accessing the published version and note that access may require a subscription. We present an experimental study of the quantum spin ice candidate pyrochlore compound Pr 2 Zr 2 O 7 by means of magnetization measurements, specific heat, and neutron scattering up to 12 T and down to 60 mK. When the field is applied along the [111] and [110] directions, k = 0 field-induced structures settle in. We find that the ordered moment rises slowly, even at very low temperature, in agreement with macroscopic magnetization. Interestingly, for H [110], the ordered moment appears on the so-called α chains only. The spin excitation spectrum is essentially inelastic and consists in a broad flat mode centered at about 0.4 meV with a magnetic structure factor which resembles the spin ice pattern. For H [110] (at least up to 2.5 T), we find that a well-defined mode forms from this broad response, whose energy increases with H , in the same way as the temperature of the specific-heat anomaly. We finally discuss these results in the light of mean field calculations and propose an interpretation where quadrupolar interactions play a major role, overcoming the magnetic exchange. In this picture, the spin ice pattern appears shifted up to finite energy because of those interactions. We then propose a range of acceptable parameters for Pr 2 Zr 2 O 7 that allow to reproduce several experimental features observed under field. With these parameters, the actual ground state of this material would be an antiferroquadrupolar liquid with spin-ice-like excitations.