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Hydrogen Vacancy Induced Superconductivity Collapse in A15 Lanthanum Hydride

Israel Osmond1, Lewis J. Conway2,3, Mikhail A. Kuzovnikov1, Callum Stevens1, Tomas Marqueño1, Hannah A. Shuttleworth1, Andrew Huxley1, Chris J. Pickard2,3, Graeme J. Ackland1 et al.

Ross T. Howie1,4 and Miriam Peña-Alvarez1,*

  • *Contact author: miriam.pena.alvarez@ed.ac.uk

Phys. Rev. Lett. 136, 086102 – Published 24 February, 2026

DOI: https://doi.org/10.1103/8b43-4dvw

Abstract

Hydrogen-rich lanthanum compounds show the highest known superconducting transition temperatures at high pressure. Despite the pivotal role of hydrogen within these systems, there has been no systematic exploration of how the composition and superconducting properties are intertwined. Our experimental and computational studies demonstrate that A15-type LaH5.75−x hosts high-Tc superconductivity (Tc=98  K at 94 GPa) when available interstitial sites are fully occupied with hydrogen. Upon decompression, a site-selective hydrogen depopulation drives a superconductor-to-insulator transition with a threshold composition of LaH5. Strikingly, the A15 framework is experimentally retained from 120 to 4 GPa, with reversible pressure-dependent hydrogen content changes from LaH5.75 down to LaH3.25. Our results demonstrate the exceptional stability and tunability of the A15 framework, offering a unique platform to probe the interplay between composition, structure, and superconductivity in hydrogen-rich materials.

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References (43)

  1. H. Liu, I. I. Naumov, Z. M. Geballe, M. Somayazulu, J. S. Tse, and R. J. Hemley, Phys. Rev. B 98, 100102(R) (2018).
  2. D. Laniel, F. Trybel, B. Winkler, F. Knoop, T. Fedotenko, S. Khandarkhaeva, A. Aslandukova, T. Meier, S. Chariton, K. Glazyrin, V. Milman, V. Prakapenka, I. A. Abrikosov, L. Dubrovinsky, and N. Dubrovinskaia, Nat. Commun. 13, 6987 (2022).
  3. J. Guo, D. Semenok, G. Shutov, D. Zhou, S. Chen, Y. Wang, K. Zhang, X. Wu, S. Luther, T. Helm, X. Huang, and T. Cui, Natl. Sci. Rev. 11, nwae149 (2024).
  4. S. Cross, J. Buhot, A. Brooks, W. Thomas, A. Kleppe, O. Lord, and S. Friedemann, Phys. Rev. B 109, L020503 (2024).
  5. F. Peng, Y. Sun, C. J. Pickard, R. J. Needs, Q. Wu, and Y. Ma, Phys. Rev. Lett. 119, 107001 (2017).
  6. M. Somayazulu, M. Ahart, A. K. Mishra, Z. M. Geballe, M. Baldini, Y. Meng, V. V. Struzhkin, and R. J. Hemley, Phys. Rev. Lett. 122, 027001 (2019).
  7. A. Drozdov, P. Kong, V. Minkov, S. Besedin, M. Kuzovnikov, S. Mozaffari, L. Balicas, F. F. Balakirev, D. Graf, V. Prakapenka et al., Nature (London) 569, 528 (2019).
  8. M. A. Kuzovnikov, A. P. Drozdov, P. P. Kong, V. S. Minkov, S. P. Besedin, V. B. Prakapenka, E. Greenberg, D. A. Knyazev, and M. I. Eremets, in 57th European High Pressure Research Group (EHPRG) Meeting on High Pressure Science and Technology (EHPRG, Prague, Czech Republic, 2019).
  9. C. Ma, Y. Ma, H. Wang, H. Wang, M. Zhou, G. Liu, and Y. Ma, J. Am. Chem. Soc. 147, 11028 (2025).
  10. D. V. Semenok, D. Zhou, A. G. Kvashnin, X. Huang, M. Galasso, I. A. Kruglov, A. G. Ivanova, A. G. Gavriliuk, W. Chen, N. V. Tkachenko, A. I. Boldyrev, I. Troyan, A. R. Oganov, and T. Cui, J. Phys. Chem. Lett. 12, 32 (2021).
  11. A. Aslandukova, A. Aslandukov, D. Laniel, Y. Yin, F. I. Akbar, M. Bykov, T. Fedotenko, K. Glazyrin, A. Pakhomova, G. Garbarino, E. L. Bright, J. Wright, M. Hanfland, S. Chariton, V. Prakapenka, N. Dubrovinskaia, and L. Dubrovinsky, Sci. Adv. 10, eadl5416 (2024).
  12. L. Ma, M. Zhou, Y. Wang, S. Kawaguchi, Y. Ohishi, F. Peng, H. Liu, G. Liu, H. Wang, and Y. Ma, Phys. Rev. Res. 3, 043107 (2021).
  13. Z. Li, X. He, C. Zhang, K. Lu, J. Zhang, S. Zhang, J. Zhao, L. Shi, Y. Peng, S. Feng et al., Chin. Phys. Lett. 42, 047401 (2025).
  14. N. P. Salke, M. M. Davari Esfahani, Y. Zhang, I. A. Kruglov, J. Zhou, Y. Wang, E. Greenberg, V. B. Prakapenka, J. Liu, A. R. Oganov et al., Nat. Commun. 10, 4453 (2019).
  15. K. Zhang, J. Yu, Y. Zhang, J. Guo, Y. Wang, C. Jiang, X. Huang, and T. Cui, J. Am. Chem. Soc. 147, 11879 (2025).
  16. E. Siska, G. A. Smith, S. Villa-Cortes, L. J. Conway, R. J. Husband, J. Van Cleave, S. Petitgirard, V. Cerantola, K. Appel, C. Baehtz et al., J. Phys. Chem. Lett. 15, 9912 (2024).
  17. M. A. Kuzovnikov, T. Hansen, A. S. Ivanov, A. I. Kolesnikov, V. I. Kulakov, S. Savvin, and M. Tkacz, Phys. Rev. B 110, 184113 (2024).
  18. D. An, W. Zhao, Q. Jiang, T. Ma, F. Tian, D. Duan, and T. Cui, Inorg. Chem. 64, 1587 (2025).
  19. D. An, D. Duan, Z. Zhang, Q. Jiang, T. Ma, Z. Huo, H. Song, and T. Cui, Phys. Rev. B 110, 054505 (2024).
  20. Y. Zhou, Y. Fu, M. Yang, I. Osmond, R. Jana, T. Nakagawa, O. Moulding, J. Buhot, S. Friedemann, D. Laniel et al., Nat. Commun. 16, 1135 (2025).
  21. V. S. Minkov, M. A. Kuzovnikov, P. Kong, A. P. Drozdov, F. Du, J. Yan, J. Kim, S. Chariton, V. B. Prakapenka, M. Mezouar, B. Wehinger, G. A. Smith, F. F. Balakirev, and E. F. Talantsev, arXiv:2507.08009.
  22. See Supplemental Material at http://link.aps.org/supplemental/10.1103/8b43-4dvw for a complete description of the experimental and computational methodology.
  23. H. Meng, M. A. Kuzovnikov, and M. Tkacz, Int. J. Hydrogen Energy 42, 29344 (2017).
  24. C. V. Storm, C. R. Roy, K. A. Munro, and M. I. McMahon, Phys. Rev. B 110, 024107 (2024).
  25. P. Loubeyre, R. LeToullec, D. Hausermann, M. Hanfland, R. J. Hemley, H. K. Mao, and L. W. Finger, Nature (London) 383, 702 (1996).
  26. C. M. Pépin, G. Geneste, A. Dewaele, M. Mezouar, and P. Loubeyre, Science 357, 382 (2017).
  27. W. Chen, D. V. Semenok, X. Huang, H. Shu, X. Li, D. Duan, T. Cui, and A. R. Oganov, Phys. Rev. Lett. 127, 117001 (2021).
  28. W. Bartscher, A. Boeuf, R. Caciuffo, J. M. Fournier, W. F. Kuhs, J. Rebizant, and F. Rustichelli, Solid State Commun. 53, 423 (1985).
  29. I. B. Magdău and G. J. Ackland, Phys. Rev. B 87, 174110 (2013).
  30. G. Ackland and I. Magdau, High Press. Res. 34, 198 (2014).
  31. M. Peña-Alvarez, J. Binns, M. Marqués, M. A. Kuzovnikov, P. Dalladay-Simpson, C. J. Pickard, G. J. Ackland, E. Gregoryanz, and R. T. Howie, J. Phys. Chem. Lett. 13, 8447 (2022).
  32. T. Marqueño, M. A. Kuzovnikov, I. Osmond, P. Dalladay-Simpson, A. Hermann, R. T. Howie, and M. Peña-Alvarez, Front. Chem. 11, 1306495 (2024).
  33. M. A. Kuzovnikov, B. Wang, X. Wang, T. Marqueño, H. A. Shuttleworth, C. Strain, E. Gregoryanz, E. Zurek, M. Peña-Alvarez, and R. T. Howie, Phys. Rev. Lett. 134, 196102 (2025).
  34. A. P. Drozdov, M. I. Eremets, I. A. Troyan, V. Ksenofontov, and S. I. Shylin, Nature (London) 525, 73 (2015).
  35. D. Sun, V. S. Minkov, S. Mozaffari, Y. Sun, Y. Ma, S. Chariton, V. B. Prakapenka, M. I. Eremets, L. Balicas, and F. F. Balakirev, Nat. Commun. 12, 6863 (2021).
  36. M. Einaga, M. Sakata, T. Ishikawa, K. Shimizu, M. I. Eremets, A. P. Drozdov, I. A. Troyan, N. Hirao, and Y. Ohishi, Nat. Phys. 12, 835 (2016).
  37. Q. Yan, X. Zhang, J. Chen, Y. Tang, Y. Ni, H. Wang, Z. Liu, and Y. Chen, J. Phys. Chem. C 128, 21551 (2024).
  38. J. Bardeen, L. N. Cooper, and J. R. Schrieffer, Phys. Rev. 108, 1175 (1957).
  39. Z. Li, X. He, C. Zhang, K. Lu, B. Min, J. Zhang, S. Zhang, J. Zhao, L. Shi, Y. Peng, S. Feng, Z. Deng, J. Song, Q. Liu, X. Wang, R. Yu, L. Wang, Y. Li, J. D. Bass, V. Prakapenka, S. Chariton, H. Liu, and C. Jin, Sci. China Phys. Mech. Astron. 66, 267411 (2023).
  40. N. P. Salke, M. M. Davari Esfahani, Y. Zhang, I. A. Kruglov, J. Zhou, Y. Wang, E. Greenberg, V. B. Prakapenka, J. Liu, A. R. Oganov, and J.-F. Lin, Nat. Commun. 10, 4453 (2019).
  41. W. Chen, X. Huang, D. V. Semenok, S. Chen, D. Zhou, K. Zhang, A. R. Oganov, and T. Cui, Nat. Commun. 14, 2660 (2023).
  42. L.-C. Chen, T. Luo, Z.-Y. Cao, P. Dalladay-Simpson, G. Huang, D. Peng, L.-L. Zhang, F. A. Gorelli, G.-H. Zhong, H.-Q. Lin, and X.-J. Chen, Nat. Commun. 15, 1809 (2024).
  43. D. V. Semenok, I. A. Troyan, A. G. Ivanova, A. G. Kvashnin, I. A. Kruglov, M. Hanfland, A. V. Sadakov, O. A. Sobolevskiy, K. S. Pervakov, I. S. Lyubutin, K. V. Glazyrin, N. Giordano, D. N. Karimov, A. L. Vasiliev, R. Akashi, V. M. Pudalov, and A. R. Oganov, Mater. Today 48, 18 (2021).

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