Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Open Access

High-pressure neutron diffraction at ultra-low temperature

Y. Wu1,*, T. E. Sherline1, J. J. Molaison1, A. M. dos Santos1, H. D. Zhou2, H. B. Cao1, J. J. Pierce1, and B. Haberl1,†

  • *Contact author: wuy1@ornl.gov
  • †Present address: Department of Materials Physics, Research School of Physics, Australian National University, Canberra, ACT 0200, Australia.

Phys. Rev. Research 7, 043063 – Published 16 October, 2025

DOI: https://doi.org/10.1103/2hx9-qjhq

Abstract

Neutron diffraction is a powerful tool in the study of quantum materials and associated emergent phenomena as it allows for direct detection of magnetic structure even at ultra-low temperatures. As pressure can drive systems across quantum critical points and tune emergent behaviors at the quantum scale, coupling neutron diffraction with extreme conditions of high pressure at (ultra-)low temperatures has been a key research target over decades. This has proven challenging as magnetic neutron diffraction typically requires large sample volumes due to flux limitations, whereas high-pressure studies require small sample volumes due to pressure limitations. Combining these two contradictory requirements poses many difficulties, but also brings opportunities in research and development. Here, we address these shortcomings through the use of a diamond anvil cell equipped with polycrystalline anvils with relatively large sample volumes coupled with the high neutron flux made available by the high-pressure diffractometer of the Spallation Neutron Source. This particular diamond anvil cell configuration has previously proven useful for single-crystal samples and is here coupled with the ultra-low temperatures of a dilution refrigerator for the first time. Our study on a single crystal of Yb2O3 successfully collected magnetic neutron diffraction data at 5.3 GPa below 200 mK inside a dilution refrigerator. We have performed a detailed analysis of the magnetic diffraction data to investigate the magnetic structure under pressure and observed a subtle shift in the transition temperature. This development will open the door for future studies on magnetic materials with these much-desired coupled extremes of high pressure and ultra-low temperatures.

View figure in article

Physics Subject Headings (PhySH)

Article Text

References (33)

  1. M. E. Zayed, C. Rüegg, J. Larrea J., A. M. Läuchli, C. Panagopoulos, S. S. Saxena, M. Ellerby, D. F. McMorrow, T. Strässle, S. Klotz, G. Hamel, R. A. Sadykov, V. Pomjakushin, M. Boehm, M. Jiménez-Ruiz, A. Schneidewind, E. Pomjakushina, M. Stingaciu, K. Conder, and H. M. Rønnow, 4-Spin plaquette singlet state in the Shastry–Sutherland compound SrCu2(BO3)2, Nat. Phys. 13, 962 (2017).
  2. E. Kermarrec, J. Gaudet, K. Fritsch, R. Khasanov, Z. Guguchia, C. Ritter, K. A. Ross, H. A. Dabkowska, and B. D. Gaulin, Ground state selection under pressure in the quantum pyrochlore magnet Yb2Ti2O7, Nat. Commun. 8, 14810 (2017).
  3. T. Hong, T. Ying, Q. Huang, S. E. Dissanayake, Y. Qiu, M. M. Turnbull, A. A. Podlesnyak, Y. Wu, H. Cao, Y. Liu, I. Umehara, J. Gouchi, Y. Uwatoko, M. Matsuda, D. A. Tennant, G.-W. Chern, K. P. Schmidt, and S. Wessel, Evidence for pressure induced unconventional quantum criticality in the coupled spin ladder antiferromagnet C9H18N2CuBr4, Nat. Commun. 13, 3073 (2022).
  4. Z. Shi, S. Dissanayake, P. Corboz, W. Steinhardt, D. Graf, D. M. Silevitch, H. A. Dabkowska, T. F. Rosenbaum, F. Mila, and S. Haravifard, Discovery of quantum phases in the Shastry-Sutherland compound SrCu2(BO3)2 under extreme conditions of field and pressure, Nat. Commun. 13, 2301 (2022).
  5. H. Sun, M. Huo, X. Hu, J. Li, Z. Liu, Y. Han, L. Tang, Z. Mao, P. Yang, B. Wang, J. Cheng, D.-X. Yao, G.-M. Zhang, and M. Wang, Signatures of superconductivity near 80 K in a nickelate under high pressure, Nature (London) 621, 493 (2023).
  6. N. Aso, T. Fujiwara, Y. Uwatoko, H. Miyano, and H. Yoshizawa, Development of a hybrid CuBe/NiCrAl clamp-type high pressure cell for neutron diffraction, J. Phys. Soc. Jpn. 76, 228 (2007).
  7. D. M. Pajerowski, A. P. Podlesnyak, J. Herbrych, and J. Manson, High-pressure inelastic neutron scattering study of the anisotropic S=1 spin chain [Ni(HF2)(3−Clpyradine)4]BF4, Phys. Rev. B 105, 134420 (2022).
  8. S. Klotz, T. Strässle, B. Lebert, M. d’Astuto, and T. Hansen, High pressure neutron diffraction to beyond 20 GPa and below 1.8 K using Paris-Edinburgh load frames, High Pressure Res. 36, 73 (2016).
  9. T. Osakabe, K. Kuwahara, D. Kawana, K. Iwasa, D. Kikuchi, Y. Aoki, M. Kohgi, and H. Sato, Pressure-induced antiferromagnetic order in filled skutterudite PrFe4P12 studied by single-crystal high-pressure neutron diffraction, J. Phys. Soc. Jpn. 79, 034711 (2010).
  10. N. Terada, D. D. Khalyavin, P. Manuel, T. Osakabe, A. Kikkawa, and H. Kitazawa, Magnetic ordering in pressure-induced phases with giant spin-driven ferroelectricity in multiferroic TbMnO3, Phys. Rev. B 93, 081104 (2016).
  11. N. Terada, N. Qureshi, A. Stunault, M. Enderle, B. Ouladdiaf, C. V. Colin, D. D. Khalyavin, P. Manuel, F. Orlandi, S. Miyahara, D. Prabhakaran, and T. Osakabe, Origin of the large ferroelectric polarization enhancement under high pressure for multiferroic DyMnO3 studied by polarized and unpolarized neutron diffraction, Phys. Rev. B 102, 085131 (2020).
  12. I. Mirebeau, I. N. Goncharenko, P. Cadavez-Peres, S. T. Bramwell, M. J. P. Gingras, and J. S. Gardner, Pressure-induced crystallization of a spin liquid, Nature (London) 420, 54 (2002).
  13. M. K. Jacobsen, C. J. Ridley, A. Bocian, O. Kirichek, P. Manuel, D. Khalyavin, M. Azuma, J. P. Attfield, and K. V. Kamenev, High-pressure cell for neutron diffraction with in situ pressure control at cryogenic temperatures, Rev. Sci. Instrum. 85, 043904 (2014).
  14. C. J. T. Ridley, Development of high pressure and cryogenic techniques, and their application to neutron diffraction, Ph.D. thesis, The University of Edinburgh, 2017.
  15. C. J. Ridley (private communication).
  16. I. Mirebeau, I. Goncharenko, H. Cao, and A. Forget, Magnetic order in Tb2Sn2O7 under high pressure: From ordered spin ice to spin liquid and antiferromagnetic order, Phys. Rev. B 80, 220407 (2009).
  17. I. Mirebeau, I. Goncharenko, and H. Cao, Spin ice and soft spin ice ground state under high pressure: Comparative study by neutron scattering, High Pressure Res. 30, 3 (2010).
  18. B. Haberl, S. Dissanayake, F. Ye, L. L. Daemen, Y. Cheng, C. W. Li, A.-J. T. Ramirez-Cuesta, M. Matsuda, J. J. Molaison, and R. Boehler, Wide-angle diamond cell for neutron scattering, High Pressure Res. 37, 495 (2017).
  19. B. Haberl, S. Dissanayake, Y. Wu, D. A. A. Myles, A. M. dos Santos, M. Loguillo, G. M. Rucker, D. P. Armitage, M. Cochran, K. M. Andrews, C. Hoffmann, H. Cao, M. Matsuda, F. Meilleur, F. Ye, J. J. Molaison, and R. Boehler, Next-generation diamond cell and applications to single-crystal neutron diffraction, Rev. Sci. Instrum. 89, 092902 (2018).
  20. S. Calder, L. An, R. Boehler, C. D. Cruz, M. Frontzek, M. Guthrie, B. Haberl, A. Huq, A. Kimber, J. Molaison, J. Neuefeind, K. Page, A. dos Santos, C. Tulk, and M. Tucker, A suite-level review of the neutron powder diffraction instruments at Oak Ridge National Laboratory, Rev. Sci. Instrum. 89, 092701 (2018).
  21. B. Haberl, M.-E. Donnelly, J. J. Molaison, M. Guthrie, and R. Boehler, Methods for neutron diffraction studies on hydride superconductors and other metal hydrides, J. Appl. Phys. 130, 215901 (2021).
  22. R. M. Moon, W. C. Koehler, H. R. Child, and L. J. Raubenheimer, Magnetic structures of Er2O3 and Yb2O3, Phys. Rev. 176, 722 (1968).
  23. H. Cao, B. C. Chakoumakos, K. M. Andrews, Y. Wu, R. A. Riedel, J. Hodges, W. Zhou, R. Gregory, B. Haberl, J. Molaison, and G. W. Lynn, DEMAND, a dimensional extreme magnetic neutron diffractometer at the high flux isotope reactor, Crystals 9, 5 (2019).
  24. R. Boehler, J. Molaison, and B. Haberl, Novel diamond cells for neutron diffraction using multi-carat CVD anvils, Rev. Sci. Instrum. 88, 083905 (2017).
  25. S. Klotz, K. Takemura, T. Strässle, and T. Hansen, Freezing of glycerol–water mixtures under pressure, J. Phys.: Condens. Matter 24, 325103 (2012).
  26. B. Haberl, J. J. Molaison, M. Frontzek, E. C. Novak, G. E. Granroth, D. Goldsby, D. C. Anderson, and A. M. Elliott, 3D-printed B4C collimation for neutron pressure cells, Rev. Sci. Instrum. 92, 093903 (2021).
  27. M. B. Stone, D. H. Siddel, A. M. Elliott, D. Anderson, and D. L. Abernathy, Characterization of plastic and boron carbide additive manufactured neutron collimators, Rev. Sci. Instrum. 88, 123102 (2017).
  28. O. Arnold et al., Mantid—data analysis and visualization package for neutron scattering and μSR experiments, Nucl. Instrum. Methods Phys. Res. Sect. A 764, 156 (2014).
  29. J. Rodríguez-Carvajal, Recent advances in magnetic-structure determination by neutron powder diffraction, Phys. B: Condens. Matter 192, 55 (1993).
  30. C. Meyer, J. P. Sanchez, J. Thomasson, and J. P. Itié, Mössbauer and energy-dispersive X-ray-diffraction studies of the pressure-induced crystallographic phase transition in C-type Yb2O3, Phys. Rev. B 51, 12187 (1995).
  31. S. Ivantchev, E. Kroumova, G. Madariaga, J. M. Perez-Mato, and M. I. Aroyo, subgroupgraph: A computer program for analysis of group-subgroup relations between space groups, J. Appl. Crystallogr. 33, 1190 (2000).
  32. I. N. Goncharenko, Neutron diffraction experiments in diamond and sapphire anvil cells, High Pressure Res. 24, 193 (2004).
  33. B. Haberl, D. G. Quirinale, C. W. Li, G. E. Granroth, H. Nojiri, M.-E. Donnelly, S. V. Ushakov, R. Boehler, and B. L. Winn, Multi-extreme conditions at the second target station, Rev. Sci. Instrum. 93, 083907 (2022).

Outline

Information

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation