Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Letter
  • Published:

Experimental signatures of emergent quantum electrodynamics in Pr2Hf2O7

Abstract

In a quantum spin liquid, the magnetic moments of the constituent electron spins evade classical long-range order to form an exotic state that is quantum entangled and coherent over macroscopic length scales1,2. Such phases offer promising perspectives for device applications in quantum information technologies, and their study can reveal new physics in quantum matter. Quantum spin ice is an appealing proposal of one such state, in which the fundamental ground state properties and excitations are described by an emergent U(1) lattice gauge theory3,4,5,6,7. This quantum-coherent regime has quasiparticles that are predicted to behave like magnetic and electric monopoles, along with a gauge boson playing the role of an artificial photon. However, this emergent lattice quantum electrodynamics has proved elusive in experiments. Here we report neutron scattering measurements of the rare-earth pyrochlore magnet Pr2Hf2O7 that provide evidence for a quantum spin ice ground state. We find a quasi-elastic structure factor with pinch points—a signature of a classical spin ice—that are partially suppressed, as expected in the quantum-coherent regime of the lattice field theory at finite temperature. Our result allows an estimate for the speed of light associated with magnetic photon excitations. We also reveal a continuum of inelastic spin excitations, which resemble predictions for the fractionalized, topological excitations of a quantum spin ice. Taken together, these two signatures suggest that the low-energy physics of Pr2Hf2O7 can be described by emergent quantum electrodynamics. If confirmed, the observation of a quantum spin ice ground state would constitute a concrete example of a three-dimensional quantum spin liquid—a topical state of matter that has so far mostly been explored in lower dimensionalities.

This is a preview of subscription content, access via your institution

Access options

Buy this article

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: Momentum dependence of magnetic correlations in Pr2Hf2O7.
Fig. 2: Line shape of the suppressed pinch points measured in Pr2Hf2O7, and comparison with model calculations.
Fig. 3: Energy spectra at fixed positions in momentum space.

Similar content being viewed by others

References

  1. Balents, L. Spin liquids in frustrated magnets. Nature 464, 199–208 (2010).

    ADS  Google Scholar 

  2. Savary, L. & Balents, L. Quantum spin liquids: a review. Rep. Prog. Phys. 80, 016502 (2016).

    ADS  Google Scholar 

  3. Hermele, M., Fisher, M. P. A. & Balents, L. Pyrochlore photons: the U(1) spin liquid in a S = ½ three-dimensional frustrated magnet. Phys. Rev. B 69, 064404 (2004).

    ADS  Google Scholar 

  4. Banerjee, A., Isakov, S. V., Damle, K. & Kim, Y.-B. Unusual liquid state of hard-core bosons on the pyrochlore lattice. Phys. Rev. Lett. 100, 047208 (2008).

    ADS  Google Scholar 

  5. Benton, O., Sikora, O. & Shannon, N. Seeing the light: experimental signatures of emergent electromagnetism in a quantum spin ice. Phys. Rev. B 86, 075154 (2012).

    ADS  Google Scholar 

  6. Gingras, M. J. P. & McClarty, P. A. Quantum spin ice: a search for gapless quantum spin liquids in pyrochlore magnets. Rep. Prog. Phys. 77, 056501 (2014).

    ADS  Google Scholar 

  7. Shannon, N., Sikora, O., Pollmann, F., Penc, K. & Fulde, P. Quantum ice: a quantum Monte Carlo study. Phys. Rev. Lett. 108, 067204 (2012).

    ADS  Google Scholar 

  8. Anderson, P. W. Resonating valence bonds: a new kind of insulator? Mat. Res. Bull. 8, 153–160 (1973).

    Google Scholar 

  9. Wen, X.-G. Quantum orders and symmetric spin liquids. Phys. Rev. B 65, 165113 (2002).

    ADS  Google Scholar 

  10. Moessner, R. & Sondhi, S. L. Resonating valence bond liquid physics on the triangular lattice. Prog. Theor. Phys. 145 (Suppl.), 37–42 (2002).

    Google Scholar 

  11. Tennant, D. A., Perring, T. G., Cowley, R. A. & Nagler, S. E. Unbound spinons in the spin-1/2 antiferromagnetic chain KCuF3. Phys. Rev. Lett. 70, 4003–4006 (1993).

    ADS  Google Scholar 

  12. Han, T.-H. et al. Fractionalized excitations in the spin-liquid state of a Kagome-lattice antiferromagnet. Nature 492, 406–410 (2012).

    ADS  Google Scholar 

  13. Banerjee, A. et al. Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet. Nat. Mater. 15, 733–740 (2016).

    ADS  Google Scholar 

  14. Shen, Y. et al. Evidence for a spinon Fermi surface in a triangular-lattice quantum-spin-liquid candidate. Nature 540, 559–562 (2016).

    ADS  Google Scholar 

  15. Castelnovo, C., Moessner, R. & Sondhi, S. L. Spin ice, fractionalization, and topological order. Annu. Rev. Condens. Matter Phys. 3, 35–55 (2012).

    Google Scholar 

  16. Bramwell, S. T. et al. Spin correlations in Ho2Ti2O7: a dipolar spin ice system. Phys. Rev. Lett. 87, 047205 (2001).

    ADS  Google Scholar 

  17. Fennell, T. et al. Magnetic Coulomb phase in the spin ice Ho2Ti2O7. Science 326, 415–417 (2009).

    ADS  Google Scholar 

  18. Henley, C. L. The “Coulomb phase” in frustrated systems. Annu. Rev. Condens. Matter Phys. 1, 179–210 (2010).

    ADS  Google Scholar 

  19. Castelnovo, C., Moessner, R. & Sondhi, S. L. Magnetic monopoles in spin ice. Nature 451, 42–45 (2008).

    ADS  Google Scholar 

  20. Curnoe, S. H. Structural distortion and the spin liquid state in Tb2Ti2O7. Phys. Rev. B 78, 094418 (2008).

    ADS  Google Scholar 

  21. Ross, K. A., Savary, L., Gaulin, B. D. & Balents, L. Quantum excitations in quantum spin ice. Phys. Rev. X 1, 021002 (2011).

    Google Scholar 

  22. Onoda, S. & Tanaka, Y. Quantum melting of spin ice: emergent cooperative quadrupole and chirality. Phys. Rev. Lett. 105, 047201 (2010).

    ADS  Google Scholar 

  23. Kimura, K. et al. Quantum fluctuations in spin-ice-like Pr2Zr2O7. Nat. Commun. 4, 1934 (2013).

    ADS  Google Scholar 

  24. Petit, S. et al. Antiferroquadrupolar correlations in the quantum spin ice candidate Pr2Zr2O7. Phys. Rev. B 94, 165153 (2016).

    ADS  Google Scholar 

  25. Wen, J.-J. et al. Disordered route to the Coulomb quantum spin liquid: random transverse fields on spin ice in Pr2Zr2O7. Phys. Rev. Lett. 118, 107206 (2017).

    ADS  Google Scholar 

  26. Martin, N. et al. Disorder and quantum spin ice. Phys. Rev. X 7, 041028 (2017).

    Google Scholar 

  27. Benton, O. From quantum spin liquid to paramagnetic ground states in disordered non-Kramers pyrochlores. Preprint at http://arXiv.org/abs/1706.09238 (2017).

  28. Sibille, R. et al. Candidate quantum spin ice in the pyrochlore Pr2Hf2O7. Phys. Rev. B 94, 024436 (2016).

    ADS  Google Scholar 

  29. Wan, Y., Carrasquilla, J. & Melko, R. G. Spinon walk in quantum spin ice. Phys. Rev. Lett. 116, 167202 (2016).

    ADS  Google Scholar 

  30. Hao, Z., Day, A. G. R. & Gingras, M. J. P. Bosonic many-body theory of quantum spin ice. Phys. Rev. B 90, 214430 (2014).

    ADS  Google Scholar 

  31. Huang, C.-J., Deng, Y., Wan Y. and Meng Z.-Y. Dynamics of topological excitations in a model quantum spin ice. Preprint at http://arXiv.org/abs/1707.00099 (2017).

  32. Savary, L. & Balents, L. Disorder-induced quantum spin liquid in spin ice pyrochlores. Phys. Rev. Lett. 118, 087203 (2017).

    ADS  Google Scholar 

  33. Chen, G. Dirac’s ‘magnetic monopoles’ in pyrochlore ice U(1) spin liquids: spectrum and classification. Phys. Rev. B 96, 195127 (2017).

    ADS  Google Scholar 

  34. Petrova, O., Moessner, R. & Sondhi, S. L. Hydrogenic states of monopoles in diluted quantum spin ice. Phys. Rev. B 92, 100401(R) (2015).

    ADS  Google Scholar 

  35. Kato, S. & Onoda, S. Numerical evidence of quantum melting of spin ice: quantum-to-classical crossover. Phys. Rev. Lett. 115, 077202 (2015).

    ADS  Google Scholar 

  36. Taillefumier, M., Benton, O., Yan, H., Jaubert, L. D. C. & Shannon, N. Competing spin liquids and hidden spin-nematic order in spin ice with frustrated transverse exchange. Phys. Rev. X 7, 041057 (2017).

    Google Scholar 

  37. Ciomaga Hatnean, M. et al. Single crystal growth, structure and magnetic properties of Pr2Hf2O7 pyrochlore. J. Phys. Condens. Matter 29, 075902 (2017).

    ADS  Google Scholar 

  38. Ollivier, J. & Mutka, H. IN5 cold neutron time-of-flight spectrometer, prepared to tackle single crystal spectroscopy. J. Phys. Soc. Jpn 80, SB003 (2011).

    Google Scholar 

  39. Ewings, R. A. et al. HORACE: Software for the analysis of data from single crystal spectroscopy experiments at time-of-flight neutron instruments. Nucl. Instrum. 834, 132–142 (2016).

    Google Scholar 

  40. Winn, B. et al. Recent progress on HYSPEC, and its polarization analysis capabilities. EPJ Web Conf. 83, 03017 (2015).

    Google Scholar 

  41. Stewart, J. R. et al. Disordered materials studied using neutron polarization analysis on the multi-detector spectrometer, D7. J. Appl. Cryst. 42, 69–84 (2009).

    Google Scholar 

  42. Isakov, S. V., Gregor, K., Moessner, R. & Sondhi, S. L. Dipolar spin correlations in classical pyrochlore magnets. Phys. Rev. Lett. 93, 167204 (2004).

    ADS  Google Scholar 

  43. Henley, C. L. Power-law spin correlations in pyrochlore antiferromagnets. Phys. Rev. B 71, 014424 (2005).

    ADS  Google Scholar 

  44. Sibille, R., Fennell, T., Gauthier, N., Kenzelmann, M. & Ollivier, J. Time-of-flight Inelastic Neutron Scattering Investigation of the Quantum Spin Ice and Quantum Kagome Ice Phases in Pr 2Hf 2O 7 (Institut Laue-Langevin, 2016); https://doi.org/10.5291/ILL-DATA.4-05-641

Download references

Acknowledgements

We acknowledge the Institut Laue-Langevin (Grenoble, France) for the allocated beamtime. We acknowledge funding from the Swiss National Science Foundation (grant nos 200021_140862; 206021_139082; and 200021_138018). This research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The work at ORNL was supported by the US DOE, Office of Science, Office of Basic Energy Sciences, under contract number DE-AC05-00OR22725. The work at the University of Warwick was supported by the EPSRC, UK, through grant EP/M028771/1. Additional neutron scattering experiments were carried out at the continuous spallation neutron source SINQ at the Paul Scherrer Institut at Villigen PSI in Switzerland.

Author information

Authors and Affiliations

Authors

Contributions

Project and experiments were designed by R.S., T.F. and M.K. Crystal growth and characterization were performed by R.S., M.C.H. and G.B. Sample alignment and mounting for the neutron scattering experiment was realized by R.S. and N.G. Neutron scattering experiments were carried out by R.S. and N.G. with J.O. and B.W. as local contacts. U.F. built the polarization neutron analyser used for the HYSPEC experiment. The experimental data were analysed by N.G., R.S., T.F. and M.K. Calculations were made by H.Y. and N.S. The paper was written by R.S. with feedback from all authors.

Corresponding author

Correspondence to Romain Sibille.

Ethics declarations

Competing interests

The authors declare no competing interests.

Additional information

Publisher’s note: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Supplementary Figures 1–4, Supplementary References

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Sibille, R., Gauthier, N., Yan, H. et al. Experimental signatures of emergent quantum electrodynamics in Pr2Hf2O7. Nature Phys 14, 711–715 (2018). https://doi.org/10.1038/s41567-018-0116-x

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41567-018-0116-x

This article is cited by

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing