- Physical Review Journals
All JournalsPhysics Magazine

Physical Review B

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
  • Letter
  • Open Access

Uranium-mercury complex antiferromagnet: UHg6.4

Yu. Prots, M. Krnel, M. Schmidt, Yu. Grin, and E. Svanidze*

  • Max-Planck-Institut für Chemische Physik fester Stoffe, Nöthnitzer Straße 40, Dresden 01187, Germany

  • *Corresponding author: svanidze@cpfs.mpg.de
PDF

Phys. Rev. B 106, L060412 – Published 31 August, 2022

DOI: https://doi.org/10.1103/PhysRevB.106.L060412

Abstract

Crystallographically complex compounds containing 4f and 5f electrons often have peculiar chemical and physical properties. In this work we present discovery and characterization of a new material UHg6.4, located at the border to complex intermetallics. This material crystallizes in the LaHg6.4 structure type, which can be represented by La/U-centered polyhedra with coordination numbers of 13 and 14. Much like the LaHg6.4 analog, UHg6.4 shows strong crystallographic disorder, in particular for Hg atoms in the channels along [001]. The UHg6.4 compound orders antiferromagnetically below TN1=35.5±1K and displays another transition at TN2=47.3±1K, which is likely also antiferromagnetic. Both transitions are only slightly affected by magnetic field. Given high air sensitivity of UHg6.4, an exceptional experimental environment for sample synthesis and characterization was necessary in order to comprehensively describe the chemical and physical properties of this system.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (78)

  1. M. H. Hamidian, A. R. Schmidt, I. A. Firmo, M. P. Allan, P. Bradley, J. D. Garrett, T. J. Williams, G. M. Luke, Y. Dubi, A. V. Balatsky, and J. C. Davis, How Kondo-holes create intense nanoscale heavy-fermion hybridization disorder, Proc. Natl. Acad. Sci. 108, 18233 (2011).
  2. G. Adrian, H. Adrian, W. Möhle, W. Gerhäuser, M. Lippert, B. Hensel, and H. Niederhofer, Irradiation induced disorder effects in heavy fermion systems, J. Magn. Magn. Mater. 76-77, 642 (1988).
  3. P. Gegenwart, F. Kromer, M. Lang, G. Sparn, C. Geibel, and F. Steglich, Non-Fermi-Liquid Effects at Ambient Pressure in a Stoichiometric Heavy-Fermion Compound with Very Low Disorder: CeNi2−zGe2, Phys. Rev. Lett. 82, 1293 (1999).
  4. R. Oishi, Y. Ohmagari, Y. Kusanose, Y. Yamane, K. Umeo, Y. Shimura, T. Onimaru, and T. Takabatake, Heavy-fermion behavior in a honeycomb Kondo lattice CePt6Al3, J. Phys. Soc. Jpn. 89, 104705 (2020).
  5. P. Swatek and D. Kaczorowski, Heavy fermion behavior in UT2Zn20 (T = Fe, Co, Ru, Rh, Ir) compounds, J. Phys. Soc. Jpn. 80, SA106 (2011).
  6. P. Gegenwart, Q. Si, and F. Steglich, Quantum criticality in heavy-fermion metals, Nat. Phys. 4, 186 (2008).
  7. F. P. Toldin, J. Figgins, S. Kirchner, and D. K. Morr, Disorder and quasiparticle interference in heavy-fermion materials, Phys. Rev. B 88, 081101(R) (2013).
  8. M. B. Tang, H. Y. Bai, W. H. Wang, D. Bogdanov, K. Winzer, K. Samwer, and T. Egami, Heavy-fermion behavior in cerium-based metallic glasses, Phys. Rev. B 75, 172201 (2007).
  9. J. C. Sarrao, C. D. Immer, C. L. Benton, Z. Fisk, and J. Lawrence, Evolution from first-order valence transition to heavy-fermion behavior, Phys. Rev. B 54, 12207 (1996).
  10. E. G. Moshopoulou, Z. Fisk, J. L. Sarrao, and J. D. Thompson, Crystal growth and intergrowth structure of the new heavy fermion materials CeIrIn5 and CeRhIn5, J. Solid State Chem. 158, 25 (2001).
  11. J. A. Mydosh, Disorder and frustration in heavy-fermion compounds, Phys. B: Condens. Matter 259-261, 882 (1999).
  12. J. L. Sarrao, C. L. Benton, Z. Fisk, J. M. Lawrence, D. Mandrus, and J. D. Thompson, YbIn1−xAgxCu4: Crossover from first-order valence transition to heavy Fermion behavior, Phys. B: Condens. Matter 223-224, 366 (1996).
  13. D. Louca, J. D. Thompson, J. M. Lawrence, R. Movshovich, C. Petrovic, J. L. Sarrao, and G. H. Kwei, Atomic disorder in the heavy fermion superconductor, Phys. Rev. B 61, R14940 (2000).
  14. W. M. Yuhasz, N. A. Frederick, P. C. Ho, N. P. Butch, B. J. Taylor, T. A. Sayles, M. B. Maple, J. B. Betts, A. H. Lacerda, P. Rogl, and G. Giester, Heavy-fermion behavior, crystalline electric field effects, and weak ferromagnetism in SmOs4Sb12, Phys. Rev. B 71, 104402 (2005).
  15. Z. Hossain, C. Geibel, T. Radu, Y. Tokiwa, F. Weickert, C. Krellner, H. Jeevan, P. Gegenwart, and F. Steglich, Low-temperature properties of the heavy fermion system YbIr2Si2, Phys. B: Condens. Matter 378-380, 74 (2006).
  16. E. Svanidze, A. Amon, R. Borth, Y. Prots, M. Schmidt, M. Nicklas, A. Leithe-Jasper, and Y. Grin, Empirical way for finding new uranium-based heavy-fermion materials, Phys. Rev. B 99, 220403(R) (2019).
  17. A. Morawski, A. Paszewin, T. Lada, and H. Marciniak, Mercury superconductors crystal growth under high pressure and high temperature influenced by crucible composition, IEEE Trans. Appl. Supercond. 7, 1903 (1997).
  18. B. Loret, A. Forget, J. B. Moussy, S. Poissonnet, P. Bonnaillie, G. Collin, P. Thuéry, A. Sacuto, and D. Colson, Crystal growth and characterization of HgBa2Ca2Cu3O8+δ superconductors with the highest critical temperature at ambient pressure, Inorg. Chem. 56, 9396 (2017).
  19. D. H. Ahmann, R. R. Baldwin, and A. S. Wilson, The uranium-mercury system (U.S. Atomic Energy Commission, Division of Technical Information, Washington, DC, 1945).
  20. R. E. Rundle and A. S. Wilson, The structures of some metal compounds of uranium, Acta Crystallogr. 2, 148 (1949).
  21. B. R. Frost, The system uranium-mercury, Vacuum 4, 368 (1954).
  22. R. Ferro, The crystal structures of ThHg3, ThIn3, ThTl3, ThSn3 and ThPb3, Acta Crystallogr. 11, 737 (1958).
  23. F. Merlo and M. L. Fornasini, Crystal structure of the R11Hg45 compounds (R = La, Ce, Pr, Nd, Sm, Gd, U), J. Less-Common Met. 64, 221 (1979).
  24. R. Domagala, R. Elliott, and W. Rostoker, The system mercury-thorium, Trans. Metall. Soc. AIME 212 (1958).
  25. C. Guminski, The Hg-Th (mercury-thorium) system, J. Phase Equilib. 15, 204 (1994).
  26. P. Ettmayer, Beitrag zum system quecksilber-thorium, Monatshefte Chem. Verwandte Teile Anderer Wissenschaften 96, 443 (1965).
  27. A. Palenzona, Th2Hg: Another representative of the CuAl2-type structure, J. Less-Common Met. 125, L5 (1986).
  28. A. Berndt, A gamma-phase in the plutonium-mercury system, J. Less-Common Met. 11, 216 (1966).
  29. A. Leithe-Jasper, H. Borrmann, and W. Hönle, Max planck institute for chemical physics of solids, Scientific report (Dresden, 2006).
  30. F. A. Rough and A. A. Bauer, Constitution of uranium and thorium alloys, Technical Report No. BMI-1300 (Battelle Memorial Inst., Columbus, Ohio, 1958).
  31. C. Guminski, The Hg-U (mercury-uranium) system, J. Phase Equilib. 24, 461 (2003).
  32. J. S. Kim and G. R. Stewart, UHg3: A heavy-fermion antiferromagnet similar to U2Zn17 and UCd11, Phys. Rev. B 89, 041103(R) (2014).
  33. Y. Prots, M. Krnel, Y. Grin, and E. Svanidze, Superconductivity in crystallographically disordered LaHg6.4, Inorganic Chemistry (to be published) (2022).
  34. WinXPow (version 2) (Darmstadt, STOE and Cie GmbH, 2001).
  35. L. Akselrud and Y. Grin, WinCSD: Software package for crystallographic calculations (Version 4), J. Appl. Crystallogr. 47, 803 (2014).
  36. See Supplemental Material at http://link.aps.org/supplemental/10.1103/PhysRevB.106.L060412 for the differential thermal analysis data, as well as magnetization data for the newly discovered UHg6.4 compound.
  37. T. S. Lee, P. Chiotti, and J. T. Mason, Phase relations in the uranium-mercury system, J. Less-Common Met. 66, 33 (1979).
  38. A. Iandelli and R. Ferro, Crystal structure of the compounds LaHg, CeHg, PrHg, and NdHg, Atti Accad. Naz. Lincei 8, 10 (1951).
  39. A. Iandelli, The structure of some ternary intermetallic compounds of the rare earths, J. Alloys Compd. 203, 137 (1994).
  40. A. V. Tkachuk and A. Mar, In search of the elusive amalgam SrHg8: A mercury-rich intermetallic compound with augmented pentagonal prisms, Dalton Trans. 39, 7132 (2010).
  41. E. Todorov and S. C. Sevov, Synthesis and structure of the alkali-metal amalgams A3Hg20 (A = Rb, Cs), K3Hg11, Cs5Hg19, and A7Hg31 (A = K, Rb), J. Solid State Chem. 149, 419 (2000).
  42. H. J. Deiseroth and E. Biehl, NaK29Hg48: A contradiction to or an extension of theoretical concepts to rationalize the structures of complex intermetallics?, J. Solid State Chem. 147, 177 (1999).
  43. E. Biehl and H. J. Deiseroth, Preparation, structural relations, and magnetism of amalgams MHg11 (M: K, Rb, Ba, Sr), Z. Anorg. Allg. Chem. 625, 1073 (1999).
  44. A. V. Tkachuk and A. Mar, Li6A17Hg9 (A = Ca, Sr, Yb): Intermetallic compounds of mercury with a zeolite-like topology of cubic networks, Chem. Eur. J. 15, 10348 (2009).
  45. J. Sappl, R. Freund, and C. Hoch, Stuck in our teeth? Crystal structure of a new copper amalgam, Cu3Hg, Crystals 7, 352 (2017).
  46. F. Tambornino and C. Hoch, The simplest representative of a complex series: The Hg-rich amalgam Yb11Hg54, Z. Kristallogr. Cryst. Mater. 232, 557 (2017).
  47. A. F. Berndt, The crystal structure of Ce5Hg21, J. Less-Common Met. 13, 366 (1967).
  48. F. Tambornino and C. Hoch, The mercury-richest Europium amalgam Eu10Hg55, Z. Anorg. Allg. Chem. 641, 537 (2015).
  49. C. Hoch and A. Simon, Cs2Hg27, das quecksilberreichste amalgam ein naher verwandter der Bergman-Phasen, Z. Anorg. Allg. Chem. 634, 853 (2008).
  50. A. V. Tkachuk and A. Mar, Alkaline-earth metal mercury intermetallics A11−xHg54+x (A = Ca, Sr), Inorg. Chem. 47, 1313 (2008).
  51. F. Tambornino and C. Hoch, Bad metal behaviour in the new Hg-rich amalgam KHg6 with polar metallic bonding, J. Alloys Compd. 618, 299 (2015).
  52. M. T. Orlando, C. A. Passos, J. L. Passamai, E. F. Medeiros, C. G. Orlando, R. V. Sampaio, H. S. Correa, F. C. De Melo, L. G. Martinez, and J. L. Rossi, Distortion of ReO6 octahedron in the Hg0.82Re0.18Ba2Ca2Cu3O8+d superconductor, Physica C 434, 53 (2006).
  53. W. Klein, R. K. Kremer, and M. Jansen, Hg2Ru2O7, a new pyrochlore showing a metal-insulator transition, J. Mater. Chem. 17, 1356 (2007).
  54. J. van Duijn, R. Ruiz-Bustos, and A. Daoud-Aladine, Kagome-like lattice distortion in the pyrochlore material Hg2Ru2O7, Phys. Rev. B 86, 214111 (2012).
  55. M. F. Mostafa, A. Hassen, and H. P. Kunkel, Irreversibility line of an Ag-doped Hg-based superconductor, Supercond. Sci. Technol. 23, 085010 (2010).
  56. N. Sakamoto, T. Akune, and U. Ruppert, AC susceptibility studies of inter-grains in Hg-1223 superconductors, J. Phys.: Conf. Ser. 97, 012067 (2008).
  57. M. Kubo, T. Akune, N. Sakamoto, H. R. Khan, and K. Lüders, Superconductivity of Ag-added composites of Hg-1223 grained Bean model, Physica C 463-465, 478 (2007).
  58. C. A. Passos, M. T. Orlando, F. D. Oliveira, P. C. Da Cruz, J. L. Passamai, C. G. Orlando, N. A. Elói, H. P. Correa, and L. G. Martinez, Effects of oxygen content on the properties of the Hg0.82Re0.18Ba2Ca2Cu3O8+d superconductor, Supercond. Sci. Technol. 15, 1177 (2002).
  59. K. Knížek, M. Veverka, E. Hadová, J. Hejtmánek, D. Sedmidubský, and E. Pollert, Synthesis of HgBa2CuO4+δ by sol-gel method under controlled oxygen pressure; Electron and thermal transport properties, Physica C: Superconductivity 302, 290 (1998).
  60. Y. Yu, Z. Y. Zeng, X. N. Xu, H. M. Shao, M. J. Qin, X. Jin, X. X. Yao, X. S. Rong, B. Ying, and Z. X. Zhao, Temperature dependence of the critical current determined from magnetic relaxation in HgBa2Ca2Cu3O8+δ, Physica C: Superconductivity 298, 240 (1998).
  61. J. Karpinski, H. Schwer, I. Mangelschots, K. Conder, A. Morawski, T. Lada, and A. Paszewin, Crystals of Hg superconductors, Nature (London) 371, 661 (1994).
  62. H. Schwer, J. Karpinski, K. Conder, L. Lesne, C. Rossel, A. Morawski, T. Lada, and A. Paszewin, X-ray single-crystal structure refinement of the 129 K superconductor HgxPb1−xBa2Ca3Cu4O10+δ, Physica C: Superconductivity 243, 10 (1995).
  63. C. T. Lin, Y. Yan, K. Peters, E. Schönherr, and M. Cardona, Flux growth of Hg1−xRexBa2Can−1CunO2n+2+δ single crystals by self-atmosphere, Physica C: Superconductivity 300, 141 (1998).
  64. R. Gatt, E. Olsson, A. Morawski, T. Lada, A. Paszewin, I. Bryntse, A. M. Grishin, Y. Eeltsev, P. Berastegui, and L. G. Johansson, Hg-1212 and Hg-1223 single crystals: Synthesis and characterisation, Physica C: Superconductivity 276, 270 (1997).
  65. J. Karpinski, 20 years high pressure materials synthesis group activity after discovery of high-Tc superconductors, in High Tc Superconductors and Related Transition Metal Oxides, edited by A. Bussmann-Holder and H. Keller (Springer-Verlag, Berlin, Heidelberg, 2007), pp. 167–175.
  66. J. Karpinski, High pressure in the synthesis and crystal growth of superconductors and IIIN semiconductors, Philos. Mag. 92, 2662 (2012).
  67. E. Biehl and H. J. Deiseroth, Rb5Hg19: Eine neue, geordnete defektvariante des BaAl4-strukturtyps, Z. Anorg. Allg. Chem. 625, 389 (1999).
  68. A. Extremera, On the surface magnetization in superconducting NaHg4, J. Less-Common Met. 134, 195 (1987).
  69. A. Extremera, The magnetic behaviour of NaHg4 peritectic, Phys. Status Solidi A 105, 281 (1988).
  70. A. Extremera, Excess molar volume and m/m* effects in the magnetic behaviour of liquid HgNa alloys, J. Phys.: Condens. Matter 3, 3663 (1991).
  71. C. Stock, J. A. Rodriguez-Rivera, K. Schmalzl, F. Demmel, D. K. Singh, F. Ronning, J. D. Thompson, and E. D. Bauer, From Ising Resonant Fluctuations to Static Uniaxial Order in Antiferromagnetic and Weakly Superconducting CeCo(In1−xHgx)5 (x=0.01), Phys. Rev. Lett. 121, 037003 (2018).
  72. W. Bao, Y. C. Gasparovic, J. W. Lynn, F. Ronning, E. D. Bauer, J. D. Thompson, and Z. Fisk, Commensurate magnetic structure of CeRhIn4.85Hg0.15, Phys. Rev. B 79, 092415 (2009).
  73. J. Tang Jr. and K. A. Gschneidner, Antiferromagnetic ordering in CeHg3, Phys. B: Condens. Matter 230-232, 186 (1997).
  74. G. Bruzzone and F. Merlo, The lanthanum-mercury system, J. Less-Common Met. 44, 259 (1976).
  75. H. H. Hill, Early Actinides: The Periodic System's f Electron Transition Metal Series,Nucl. Met., Met. Soc. AIME 17, 2 (1970).
  76. A. Misiuk, J. Mulak, A. Czopnik, and W. Trzebiatowski, Magnetic properties of some uranium compounds of the AlB2 type, Bull. Acad. Pol. Sci. 20, 337 (1972).
  77. V. Sechovsky and L. Havela, Intermetallic Compounds of Actinides, Handbook of Ferromagnetic Materials, Vol. 4 (Elsevier Science, Amsterdam, 1988), pp. 309–491.
  78. Z. Fisk, H. R. Ott, and J. L. Smith, Chemical physics of heavy electron uranium compounds, J. Less-Common Met. 133, 99 (1987).

Outline

Information

Phys. Rev. B 106, L060412– Published 31 August, 2022
  • Received 31 March 2022
  • Revised 8 July 2022
  • Accepted 22 August 2022
Crossmark - Check for updates button
Creative Commons Logo

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI. Open access publication funded by the Max Planck Society.

Published by the American Physical Society

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation