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A Perspective on Conventional High-Temperature Superconductors at High Pressure: Methods and Materials

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 Publication date 2019
  fields Physics
and research's language is English




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Two hydrogen-rich materials, H$_3$S and LaH$_{10}$, synthesized at megabar pressures, have revolutionized the field of condensed matter physics providing the first glimpse to the solution of the hundred-year-old problem of room temperature superconductivity. The mechanism underlying superconductivity in these exceptional compounds is the conventional electron-phonon coupling. Here we describe recent advances in experimental techniques, superconductivity theory and first-principles computational methods which have made possible these discoveries. This work aims to provide an up-to-date compendium of the available results on superconducting hydrides and explain how the synergy of different methodologies led to extraordinary discoveries in the field. Besides, in an attempt to evidence empirical rules governing superconductivity in binary hydrides under pressure, we discuss general trends in the electronic structure and chemical bonding. The last part of the Review introduces possible strategies to optimize pressure and transition temperatures in conventional superconducting materials as well as future directions in theoretical, computational and experimental research.



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We survey the landscape of binary hydrides across the entire periodic table from 10 to 500 GPa using a crystal structure prediction method. Building a critical temperature ($T_c$) model, with inputs arising from density of states calculations and Gaspari-Gyorffy theory, allows us to predict which energetically competitive candidates are most promising for high-$T_c$ superconductivity. Implementing optimisations, which lead to an order of magnitude speed-up for electron-phonon calculations, then allows us to perform an unprecedented number of high-throughput calculations of $T_c$ based on these predictions and to refine the model in an iterative manner. Converged electron-phonon calculations are performed for 121 of the best candidates from the final model. From these, we identify 36 above-100 K dynamically stable superconductors. To the best of our knowledge, superconductivity has not been previously studied in 27 of these. Of the 36, 18 exhibit superconductivity above 200 K, including structures of NaH$_6$ (248-279 K) and CaH$_6$ (216-253 K) at the relatively low pressure of 100 GPa.
In this work, we show that the same theoretical tools that successfully explain other hydrides systems under pressure seem to be at odds with the recently claimed conventional room temperature superconductivity of the carbonaceous sulfur hydride. We support our conclusions with I) the absence of a dominant low-enthalpy stoichiometry and crystal structure in the ternary phase diagram. II) Only the thermodynamics of C-doping phases appears to be marginally competing in enthalpy against H$_3$S. III) Accurate results of the transition temperature given by ab initio Migdal-Eliashberg calculations differ by more than 110 K to recently theoretical claims explaining the high-temperature superconductivity in carbonaceous-hydrogen sulfide. A novel mechanism of superconductivity or a breakdown of current theories in this system is possibly behind the disagreement.
Due to its low atomic mass hydrogen is the most promising element to search for high-temperature phononic superconductors. However, metallic phases of hydrogen are only expected at extreme pressures (400 GPa or higher). The measurement of a record superconducting critical temperature of 190 K in a hydrogen-sulfur compound at 200 GPa of pressure[1], shows that metallization of hydrogen can be reached at significantly lower pressure by inserting it in the matrix of other elements. In this work we re-investigate the phase diagram and the superconducting properties of the H-S system by means of minima hopping method for structure prediction and Density Functional theory for superconductors. We also show that Se-H has a similar phase diagram as its sulfur counterpart as well as high superconducting critical temperature. We predict SeH3 to exceed 120 K superconductivity at 100 GPa. We show that both SeH3 and SH3, due to the critical temperature and peculiar electronic structure, present rather unusual superconducting properties.
Superconductivity was discovered in 1911 by Kamerlingh Onnes and Holst in mercury at the temperature of liquid helium (4.2 K). It took almost 50 years until in 1957 a microscopic theory of superconductivity, the so-called BCS theory, was developed. Since the discovery a number of superconducting materials were found with transition temperatures up to 23 K. A breakthrough in the field happened in 1986 when Bednorz and Muller discovered a new class of superconductors, the so-called cuprate high-temperature superconductors with transition temperatures as high as 135 K. This surprising discovery initiated new efforts with respect to fundamental physics, material science, and technological applications. In this brief review the basic physics of the conventional low-temperature superconductors as well as of the high-temperature superconductors are presented with a brief introduction to applications exemplified from high-power to low-power electronic devices. Finally, a short outlook and future challenges are presented, finished with possible imaginations for applications of room-temperature superconductivity.
Universal scaling laws can guide the understanding of new phenomena, and for cuprate high-temperature superconductivity such an early influential relation showed that the critical temperature of superconductivity ($T_c$) correlates with the density of the superfluid measured at low temperatures. This famous Uemura relation has been inspiring the community ever since. Here we show that the charge content of the bonding orbitals of copper and oxygen in the ubiquitous CuO$_2$ plane, accessible with nuclear magnetic resonance (NMR), is tied to the Uemura scaling. This charge distribution between copper and oxygen varies between cuprate families and with doping, and it allows us to draw a new phase diagram that has different families sorted with respect to their maximum $T_c$. Moreover, it also shows that $T_c$ could be raised substantially if we were able to synthesize materials in which more oxygen charge is transferred to the approximately half filled copper orbital.
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