skip to main content


Title: High-temperature superconductivity on the verge of a structural instability in lanthanum superhydride
Abstract

The possibility of high, room-temperature superconductivity was predicted for metallic hydrogen in the 1960s. However, metallization and superconductivity of hydrogen are yet to be unambiguously demonstrated and may require pressures as high as 5 million atmospheres. Rare earth based “superhydrides”, such as LaH10, can be considered as a close approximation of metallic hydrogen even though they form at moderately lower pressures. In superhydrides the predominance of H-H metallic bonds and high superconducting transition temperatures bear the hallmarks of metallic hydrogen. Still, experimental studies revealing the key factors controlling their superconductivity are scarce. Here, we report the pressure and magnetic field dependence of the superconducting order observed in LaH10. We determine that the high-symmetry high-temperature superconductingFm-3mphase of LaH10can be stabilized at substantially lower pressures than previously thought. We find a remarkable correlation between superconductivity and a structural instability indicating that lattice vibrations, responsible for the monoclinic structural distortions in LaH10, strongly affect the superconducting coupling.

 
more » « less
NSF-PAR ID:
10360416
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ;
Publisher / Repository:
Nature Publishing Group
Date Published:
Journal Name:
Nature Communications
Volume:
12
Issue:
1
ISSN:
2041-1723
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    The discovery of superconductivity at 260 K in hydrogen-rich compounds like LaH10re-invigorated the quest for room temperature superconductivity. Here, we report the temperature dependence of the upper critical fieldsμ0Hc2(T) of superconducting H3S under a record-high combination of applied pressures up to 160 GPa and fields up to 65 T. We find thatHc2(T) displays a linear dependence on temperature over an extended range as found in multigap or in strongly-coupled superconductors, thus deviating from conventional Werthamer, Helfand, and Hohenberg (WHH) formalism. The best fit ofHc2(T) to the WHH formalism yields negligible values for the Maki parameterαand the spin–orbit scattering constantλSO. However,Hc2(T) is well-described by a model based on strong coupling superconductivity with a coupling constantλ~ 2. We conclude that H3S behaves as a strong-coupled orbital-limited superconductor over the entire range of temperatures and fields used for our measurements.

     
    more » « less
  2. The search for room temperature superconductivity has accelerated in the last few years driven by experimentally accessible theoretical predictions that indicated alloying dense hydrogen with other elements could produce conventional superconductivity at high temperatures and pressures. These predictions helped inform the synthesis of simple binary hydrides that culminated in the discovery of the superhydride LaH 10 with a superconducting transition temperature T c of 260 K at 180 GPa. We have now successfully synthesized a metallic La-based superhydride with an initial T c of 294 K. When subjected to subsequent thermal excursions that promoted a chemical reaction to a higher order system, the T c onset was driven irreversibly to 556 K. X-ray characterization confirmed the formation of a distorted LaH 10 based backbone that suggests the formation of ternary or quaternary compounds with substitution at the La and/or H sites. The results provide evidence for hot superconductivity, aligning with recent predictions for higher order hydrides under pressure. 
    more » « less
  3. Abstract

    Following the discovery of high-temperature superconductivity in the La–H system, we studied the formation of new chemical compounds in the barium-hydrogen system at pressures from 75 to 173 GPa. Using in situ generation of hydrogen from NH3BH3, we synthesized previously unknown superhydride BaH12with a pseudocubic (fcc) Ba sublattice in four independent experiments. Density functional theory calculations indicate close agreement between the theoretical and experimental equations of state. In addition, we identified previously knownP6/mmm-BaH2and possibly BaH10and BaH6as impurities in the samples. Ab initio calculations show that newly discovered semimetallic BaH12contains H2and H3molecular units and detached H12chains which are formed as a result of a Peierls-type distortion of the cubic cage structure. Barium dodecahydride is a unique molecular hydride with metallic conductivity that demonstrates the superconducting transition around 20 K at 140 GPa.

     
    more » « less
  4. Abstract

    Since the discovery of superconductivity at ~ 200 K in H3S [1], similar or higher transition temperatures,Tcs, have been reported for various hydrogen-rich compounds under ultra-high pressures [2]. Superconductivity was experimentally proved by different methods, including electrical resistance, magnetic susceptibility, optical infrared, and nuclear resonant scattering measurements. The crystal structures of superconducting phases were determined by X-ray diffraction. Numerous electrical transport measurements demonstrate the typical behavior of a conventional phonon-mediated superconductor: zero resistance belowTc, shift ofTcto lower temperatures under external magnetic fields, and pronounced isotope effect. Remarkably, the results are in good agreement with the theoretical predictions, which describe superconductivity in hydrides within the framework of the conventional BCS theory. However, despite this acknowledgement, experimental evidences for the superconducting state in these compounds have recently been treated with criticism [3–7], which apparently stems from misunderstanding and misinterpretation of complicated experiments performed under very high pressures. Here, we describe in greater detail the experiments revealing high-temperature superconductivity in hydrides under high pressures. We show that the arguments against superconductivity [3–7] can be either refuted or explained. The experiments on the high-temperature superconductivity in hydrides clearly contradict the theory of hole superconductivity [8] and eliminate it [3].

     
    more » « less
  5. Abstract

    The high critical superconducting temperatures (Tcs) of metal hydride phases with clathrate‐like hydrogen networks have generated great interest. Herein, we employ the Density Functional Theory‐Chemical Pressure (DFT‐CP) method to explain why certain electropositive elements adopt these structure types, whereas others distort the hydrogenic lattice, thereby decreasing theTc. The progressive opening of the H24polyhedra in MH6phases is shown to arise from internal pressures exerted by large metal atoms, some of which may favor an even higher hydrogen content that loosens the metal atom coordination environments. The stability of the LaH10and LaBH8phases is tied to stuffing of their shared hydrogen network with either additional hydrogen or boron atoms. The predictive capabilities of DFT‐CP are finally applied to the Y−X−H system to identify possible ternary additions yielding a superconducting phase stable to low pressures.

     
    more » « less