Abstract
Liquids are expected to crystallize at low temperature. The only exception is helium, which can remain liquid at 0 K, owing to quantum fluctuations1,2. Similarly, the atomic magnetic moments (spins) in a magnet are expected to order at a temperature scale set by the Curie–Weiss temperature θCW (ref. 3). Geometrically frustrated magnets represent an exception. In these systems, the pairwise spin interactions cannot be simultaneously minimized because of the lattice symmetry4. This can stabilize a liquid-like state of short-range-ordered fluctuating moments well below θCW (refs 5–7). Here we use neutron scattering to observe the spin liquid state in a geometrically frustrated system, Tb2Ti2O7, under conditions of high pressure (∼9 GPa) and low temperature (∼1 K). This compound is a three-dimensional magnet with θCW = -19 K, where the negative value indicates antiferromagnetic interactions. At ambient pressure Tb2Ti2O7 remains in a spin liquid state down to at least 70 mK (ref. 8). But we find that, under high pressure, the spins start to order or ‘crystallize’ below 2.1 K, with antiferromagnetic order coexisting with liquid-like fluctuations. These results indicate that a spin liquid/solid mixture can be induced by pressure in geometrically frustrated systems.
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References
Keeson, W. H. Helium (Elsevier, Amsterdam, 1942)
Simon, F. E. & Swenson, C. A. The liquid–solid transition in helium near absolute zero. Nature 165, 829–831 (1950)
Morrish, A. The Physical Principles of Magnetism (Wiley & Sons, New York, 1965)
Reimers, J. N., Berlinsky, A. J. & Shi, A. C. Mean-field approach to magnetic ordering in highly frustrated pyrochlores. Phys. Rev. B 43, 865–878 (1991)
Lee, S.-H. et al. Isolated spin pairs and two-dimensional magnetism in SrCr9pGa12–9pO19 . Phys. Rev. Lett. 76, 4424–4427 (1996)
Schiffer, P., Ramirez, A. P., Huse, D. A. & Valentino, A. J. Investigation of the field induced antiferromagnetic phase transition in the frustrated magnet: gadolinium gallium garnet. Phys. Rev. Lett. 73, 2500–2503 (1994)
Petrenko, O. A., Ritter, C., Yethiraj, M. & Paul, D. McK. Investigation of the low-temperature spin-liquid behavior of the frustrated magnet gadolinium gallium garnet. Phys. Rev. Lett. 80, 4570–4573 (1998)
Gardner, J. S. et al. Cooperative paramagnetism in the geometrically frustrated pyrochlore antiferromagnet Tb2Ti2O7 . Phys. Rev. Lett. 82, 1012–1015 (1999)
Bramwell, S. T. & Gingras, M. J. P. Spin ice state in frustrated magnetic pyrochlore materials. Science 294, 1495–1501 (2001)
Champion, J. D. M. et al. Er2Ti2O7: Evidence of order by disorder in a frustrated quantum antiferromagnet. Phys. Rev. Lett. (2001) (submitted); preprint cond-mat/0112007 at 〈http://xxx.lanl.gov〉
Palmer, S. E. & Chalker, J. T. Order induced by dipolar interactions in a geometrically frustrated antiferromagnet. Phys. Rev. B. 62, 488–492 (2000)
Ferey, G., de Pape, R., Leblanc, M. & Pannetier, J. Ordered magnetic frustration: VIII. Crystal and magnetic structures of the pyrochlore form of FeF3 between 2.5 and 25 K from powder neutron diffraction. Comparison with the other varieties of FeF3 . Rev. Chim. Minér. 23, 474–484 (1986)
Champion, J. D. M. et al. Order in the Heisenberg pyrochlore: The magnetic structure of Gd2Ti2O7 . Phys. Rev. B 64, 140407 (2001)
Gaulin, B. D., Reimers, J. N., Mason, T. E., Greedan, J. E. & Tun, Z. Spin freezing in the geometrically frustrated pyrochlore Tb2Mo2O7 . Phys. Rev. Lett. 69, 3244–3247 (1992)
Luo, G., Hess, S. T. & Corruccini, L. R. Low temperature magnetic properties of the geometrically frustrated pyrochlores Tb2Ti2O7, Gd2Ti2O7, Gd2Sn2O7 . Phys. Lett. A 291, 306–310 (2001)
Gingras, M. J. P. et al. Thermodynamic and single-ion properties of Tb3+ within the collective paramagnetic-spin liquid state of the frustrated pyrochlore antiferromagnet Tb2Ti2O7 . Phys. Rev. B 62, 6496–6511 (2000)
Yasui, Y. et al. Static correlation and dynamical properties of Tb3+ moments in Tb2Ti2O7—Neutron scattering study. J. Phys. Soc. Jpn 71, 599–609 (2002)
den Hertog, B. C. & Gingras, M. J. P. Dipolar interactions and origin of spin ice in Ising pyrochlore magnets. Phys. Rev. Lett. 84, 3430–3433 (2000)
Kao, Y. J., Enjalran, M. & Gingras, M. J. P. Understanding paramagnetic correlations in the spin-liquid pyrochlore Tb2Ti2O7. Preprint cond-mat/0207270 at 〈http://xxx.lanl.gov〉 (2002).
Goncharenko, I. N., Glazkov, V. P., Irodova, A. V., Lavrova, O. A. & Somenkov, V. A. Compressibility of dihydrides of transition metals. J. Alloys Comp. 179, 253–257 (1992)
Goncharenko, I. N. & Mirebeau, I. Magnetic neutron diffraction under very high pressures. Study of europium monochalcogenides. Rev. High Press. Sci. Technol. 7, 475–480 (1998)
Rodríguez-Carvajal, J. Recent advances in magnetic structure determination by neutron powder diffraction. Physica B 192, 55–69 (1993)
Greedan, J. E., Reimers, J. N., Stager, C. V. & Penny, S. L. Neutron-diffraction study of magnetic ordering in the pyrochlore series R2Mo2O7 (R = Nd,Tb,Y). Phys. Rev B 43, 5682–5691 (1991)
Tsui, Y. K., Snyder, J. & Schiffer, P. Analog to the 4He melting curve in a model geometrically frustrated magnet. Can. J. Phys. 79, 1439–1446 (2001)
Reimers, J. N. Diffuse-magnetic-scattering calculations for frustrated antiferromagnets. Phys. Rev. B 46, 193–202 (1992)
Canals, B. & Garanin, D. A. Spin liquid phase in the pyrochlore antiferromagnet. Can. J. Phys. 79, 1323–1331 (2001)
Acknowledgements
We thank J. Rodríguez-Carvajal for help in the structural analysis, and J. Hodges for discussions. P.C.-P. was supported by Fundação para a Ciência e a Tecnologia, Portugal; M.G. was supported by NSERC of Canada, the Province of Ontario and Research Corporation.
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Mirebeau, I., Goncharenko, I., Cadavez-Peres, P. et al. Pressure-induced crystallization of a spin liquid. Nature 420, 54–57 (2002). https://doi.org/10.1038/nature01157
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DOI: https://doi.org/10.1038/nature01157
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