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Antiferroquadrupolar correlations in the quantum spin ice candidate Pr2Zr2O7

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Petit, S., Lhotel, E., Guitteny, S., Florea, O., Robert, J., Bonville, P., Mirebeau, I., Ollivier, J., Mutka, H., Ressouche, E., Decorse, C., Ciomaga Hatnean, Monica and Balakrishnan, Geetha (2016) Antiferroquadrupolar correlations in the quantum spin ice candidate Pr2Zr2O7. Physical Review B, 94 (16). 165153 . doi:10.1103/PhysRevB.94.165153 ISSN 2469-9950.

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Official URL: http://dx.doi.org/10.1103/PhysRevB.94.165153

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Abstract

We present an experimental study of the quantum spin ice candidate pyrochlore compound Pr2Zr2O7 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 [1-10] 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 // [1-10], 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 // [1-10] (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 Pr2Zr2O7 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.

Item Type: Journal Article
Subjects: Q Science > QC Physics
Divisions: Faculty of Science, Engineering and Medicine > Science > Physics
Library of Congress Subject Headings (LCSH): Nuclear spin, Crystal field theory, Antiferromagnetism
Journal or Publication Title: Physical Review B
Publisher: American Physical Society
ISSN: 2469-9950
Official Date: 21 October 2016
Dates:
DateEvent
21 October 2016Published
5 September 2016Accepted
Volume: 94
Number: 16
Article Number: 165153
DOI: 10.1103/PhysRevB.94.165153
Status: Peer Reviewed
Publication Status: Published
Access rights to Published version: Restricted or Subscription Access
Copyright Holders: American Physical Society
Date of first compliant deposit: 24 April 2017
Date of first compliant Open Access: 25 April 2017
Funder: Engineering and Physical Sciences Research Council (EPSRC)
Grant number: EP/M028771/1

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