First-principles search of hot superconductivity in La-X-H ternary hydrides
Source abstract
Abstract
Abstract Motivated by the recent claim of hot superconductivity with critical temperatures up to 550 K in La + x hydrides, we investigate the high-pressure phase diagram of compounds that may have formed in the experiment, using first-principles calculations for evolutionary crystal structure prediction and superconductivity. Starting from the hypothesis that the observed Tc may be realized by successive heating upon a pre-formed LaH10 phase, we examine plausible ternaries of lanthanum, hydrogen and other elements present in the diamond anvil cell: boron, nitrogen, carbon, platinum, gallium, gold. We find that only boron and, to a lesser extent, gallium form metastable superhydride-like structures that can host high-Tc superconductivity, but the predicted Tc’s are incompatible with the experimental reports. Our results indicate that, while the claims of hot superconductivity should be reconsidered, it is very likely that unknown H-rich ternary or multinary phases containing lanthanum, hydrogen, and possibly boron or gallium may have formed under the reported experimental conditions, and that these may exhibit superconducting properties comparable, or even superior, to those of currently known hydrides.
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Research context
OpenAlex topics: High-pressure geophysics and materials · Rare-earth and actinide compounds · Diamond and Carbon-based Materials Research
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (48)
Show source-provided references
1. Einaga, M. et al. Crystal structure of the superconducting phase of sulfur hydride. Nat. Phys. 12, 835–838 (2016).10.1038/nphys3760 ↗
2. Duan, D. et al. Pressure-induced metallization of dense (S2H)2H2 with high-Tc superconductivity. Sci. Rep. 4, 6968 (2014).10.1038/srep06968 ↗
3. Zurek, E. & Bi, T. High-temperature superconductivity in alkaline and rare-earth polyhydrides at high pressure: a theoretical perspective. J. Chem. Phys. 150, 050901 (2019).10.1063/1.5079225 ↗
4. Flores-Livas, J. A. et al. A perspective on conventional high-temperature superconductors at high pressure: Methods and materials. Phys. Rep. 856, 1–78 (2020).10.1016/j.physrep.2020.02.003 ↗
5. Semenok, D. V., Kruglov, I. A., Savkin, I. A., Kvashin, A. G. & Oganov, A. R. On distribution of superconductivity in metal hydrides. Curr. Opin. Solid State Mater. Sci. 24, 100808 (2020).10.1016/j.cossms.2020.100808 ↗
6. Drodzov, A. P. et al. Superconductivity at 250 K in lanthanum hydride under high pressure. Nature 569, 528–531 (2019).10.1038/s41586-019-1201-8 ↗
7. Somayazulu, M. et al. Evidence for superconductivity above 260 K in lanthanum superhydride at megabar pressures. Phys. Rev. Lett. 122, 027001 (2019).10.1103/PhysRevLett.122.027001 ↗
8. Liu, H., Naumov, I. I., Hoffmann, R., Ashcroft, N. W. & Hemley, R. J. Potential high-Tc superconducting lanthanum and yttrium hydrides at high pressure. PNAS 114, 6990–6995 (2017).10.1073/pnas.1704505114 ↗
9. Semenok, D. V. et al. Superconductivity at 161 K in thorium hydride thh10: synthesis and properties. Mat. Tod. 33, 36–44 (2020).10.1016/j.mattod.2019.10.005 ↗
10. Troyan, I. A. et al. Anomalous high-temperature superconductivity in YH6. Adv. Mater. 33, 2006832 (2021).10.1002/adma.202006832 ↗
11. Kong, P. P. et al. Superconductivity up to 243 K in yttrium hydrides under high pressure. Nat. Comm. 12, 5075 (2021).10.1038/s41467-021-25372-2 ↗
12. Drodzov, A. P., Eremets, M. I. & Troyan, I. A. Superconductivity above 100 K in PH3 at high pressures. Preprint at https://arxiv.org/abs/1508.06224 (2015).
13. Snider, E. et al. Room-temperature superconductivity in a carbonaceous sulfur hydride. Nature 586, 373–377 (2020).10.1038/s41586-020-2801-z ↗
14. Sun, Y., Lv, J., Xie, Y., Liu, H. & Ma, Y. Route to a superconducting phase above room temperature in electron-doped hydride compounds under high pressure. Phys. Rev. Lett. 123, 097001 (2019).10.1103/PhysRevLett.123.097001 ↗
15. Grockowiak, A. D. et al. Hot hydride superconductivity above 550 K. Preprint at https://arxiv.org/abs/2006.03004 (2020).
16. Boeri, L. & Bachelet, G. B. Viewpoint: the road to room-temperature conventional superconductivity. J. Phys.: Condens. Matter 31, 234002 (2019).
17. Shipley, A. M., Hutcheon, M. J., Needs, R. J. & Pickard, C. J. High-throughput discovery of high-temperature conventional superconductors. Phys. Rev. B 104, 054501 (2021).10.1103/PhysRevB.104.054501 ↗
18. Errea, I. et al. Quantum hydrogen-bond symmetrization in the superconducting hydrogen sulfide system. Nature 532, 81–84 (2016).10.1038/nature17175 ↗
19. Errea, I. et al. Quantum crystal structure in the 250-Kelvin superconducting lanthanum hydride. Nature 578, 66–69 (2020).10.1038/s41586-020-1955-z ↗
20. Zurek, E., Hoffmann, R., Ashcroft, N. W., Oganov, A. R. & Lyakhov, A. O. A little bit of lithium does a lot for hydrogen. PNAS 106, 17640–17643 (2009).10.1073/pnas.0908262106 ↗
21. Peng, F. et al. Hydrogen clathrate structures in rare earth hydrides at high pressures: possible route to room-temperature superconductivity. Phys. Rev. Lett. 119, 107001 (2017).10.1103/PhysRevLett.119.107001 ↗
22. Glass, C. W., Oganov, A. R. & Hansen, N. USPEX–evolutionary crystal structure prediction. Comput. Phys. Commun. 175, 713–720 (2006).10.1016/j.cpc.2006.07.020 ↗
23. Lyakhov, A. O., Oganov, A. R., Stokes, H. T. & Zhu, Q. New developments in evolutionary structure prediction algorithm uspex. Comput. Phys. Commun. 184, 1172–1182 (2013).10.1016/j.cpc.2012.12.009 ↗
24. Teredesai, P. et al. High pressure phase transition in metallic LaB6: Raman and x-ray diffraction studies. Solid State Comm. 129 (2004).10.1016/j.ssc.2003.12.041 ↗
25. Cava, R. J. et al. Superconductivity in lanthanum nickel boro-nitride. Nature 273, 245–247 (1994).10.1038/372245a0 ↗
26. Cataldo, S. D., von der Linden, W. & Boeri, L. Phase diagram and superconductivity of calcium borohydrides at extreme pressures. Phys. Rev. B 102, 014516 (2020).10.1103/PhysRevB.102.014516 ↗
27. Kokail, C., von der Linden, W. & Boeri, L. Prediction of high-tc conventional superconductivity in the ternary lithium borohydride system. Phys. Rev. M 1, 074803 (2017).
28. Liang, X. et al. Prediction of high-Tc superconductivity in ternary lanthanum borohydrides. Phys. Rev. B, 134501 (2021).
29. Belli, F., Novoa, T., Contreras-Garcia, J. & Errea, I. Strong correlation between bonding network and critical temperature in hydrogen-based superconductors. Nat. Commun. 12, 1–11 (2021).10.1038/s41467-021-25687-0 ↗
30. Borinaga, M., Errea, I., Calandra, M., Mauri, F. & Bergara, A. Anharmonic effects in atomic hydrogen: Superconductivity and lattice dynamical stability. Phys. Rev. B 93, 174308 (2016).10.1103/PhysRevB.93.174308 ↗
31. Azadi, S., Monserrat, B., Foulkes, W. M. C. & Needs, R. J. Dissociation of high-pressure solid molecular hydrogen: a quantum monte carlo and anharmonic vibrational study. Phys. Rev. Lett. 112, 165501 (2014).10.1103/PhysRevLett.112.165501 ↗
32. Allen, P. B. & Dynes, R. C. Transition temperature of strong-coupled superconductors reanalyzed. Phys. Rev. B 12, 905 (1975).10.1103/PhysRevB.12.905 ↗
33. Carbotte, J. P. Properties of boson-exchange superconductorsa. Rev. Mod. Phys. 62, 1027 (1990).10.1103/RevModPhys.62.1027 ↗
34. Heil, C., Cataldo, S. D., Bachelet, G. B. & Boeri, L. Superconductivity in sodalite-like yttrium hydrides. Phys. Rev. B 99, 220502(R) (2019).10.1103/PhysRevB.99.220502 ↗
35. Cataldo, S. D., Heil, C., von der Linden, W. & Boeri, L. LaBH8: towards high-tc low-pressure superconductivity in ternary superhydrides. Phys. Rev. B 104, L020511 (2021).
36. Zhang, Z. et al. Design principles for high temperature superconductors with hydrogen-based alloy backbone at moderate pressure. Preprint at https://arxiv.org/abs/2106.09879 (2021).
37. Kresse, G. & Furthmüller, J. Efficient iterative schemes for ab-initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 54, 11169 (1996).10.1103/PhysRevB.54.11169 ↗
38. Kvashin, A. G., Tantardini, C., Zakaryan, H. A., Kvashina, Y. A. & Oganov, A. R. Computational search for new w-mo-b compounds. Chem. Mater. 32, 7028–7035 (2020).10.1021/acs.chemmater.0c02440 ↗
39. Ong, S. P. et al. Python materials genomics (pymatgen): a robust, open-source python library for materials analysis. Comput. Mater. Sci. 68, 314–319 (2013).10.1016/j.commatsci.2012.10.028 ↗
40. Zhou, X.-F. et al. Superconducting high-pressure phase of platinum hydride from first principles. Phys. Rev. B 84, 054543 (2011).10.1103/PhysRevB.84.054543 ↗
41. Hu, C.-H. et al. Pressure-induced stabilization and insulator-superconductor transition of BH. Phys. Rev. Lett. 110, 165504 (2013).10.1103/PhysRevLett.110.165504 ↗
42. Pickard, C. J. & Needs, R. J. Highly compressed ammonia forms an ionic crystal. Nat. Mater. 775–779 (2008).10.1038/nmat2261 ↗
43. Momma, K. & Izumi, F. Vesta: a three-dimensional visualization system for electronic and structural analysis. J. Appl. Cryst. 41, 653–658 (2008).10.1107/S0021889808012016 ↗
44. Giannozzi, P. et al. Quantum espresso: a modular and open-source software project for quantum simulation of materials. J. Phys. Condens. Matter 21, 395502 (2009).10.1088/0953-8984/21/39/395502 ↗
45. Baroni, S., de Gironcoli, S., Corso, A. D. & Giannozzi, P. Phonons and related crystal properties from density-functional perturbation theory. Rev. Mod. Phys. 73, 515 (2001).10.1103/RevModPhys.73.515 ↗
46. Savrasov, S. Y. & Savrasov, D. Y. Electron-phonon interactions and related physical properties of metals from linear-response theory. Phys. Rev. B 54, 16487 (1990).10.1103/PhysRevB.54.16487 ↗
47. Giannozzi, P. et al. Advanced capabilities for materials modelling with quantum espresso. J. Phys. Condens. Matter 29, 465901 (2017).10.1088/1361-648X/aa8f79 ↗
48. Hamann, D. R. Optimized norm-conserving Vanderbilt pseudopotentials. Phys. Rev. B 88, 085117 (2017).10.1103/PhysRevB.88.085117 ↗