skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Search for: All records

Award ID contains: 2104881

Note: When clicking on a Digital Object Identifier (DOI) number, you will be taken to an external site maintained by the publisher. Some full text articles may not yet be available without a charge during the embargo (administrative interval).
What is a DOI Number?

Some links on this page may take you to non-federal websites. Their policies may differ from this site.

  1. Abstract Understanding how microscopic structural domains govern macroscopic electronic properties is central to advancing hydride superconductors, yet such correlations remain poorly resolved under pressure. We report the synthesis and characterization of (La0.9Y0.1)H10superhydrides exhibiting coexisting cubic$${Fm}\bar{3}m$$ F m 3 ¯ m and hexagonal$$P{6}_{3}/{mmc}$$ P 6 3 / m m c clathrate phases observed over the pressure range from 168 GPa down to 136 GPa. Using synchrotron-based X-ray diffraction imaging at the upgraded Advanced Photon Source, we spatially resolved μm-scale distributions of these phases, revealing structural inhomogeneity across the sample. Four-probe resistance measurements confirmed superconductivity with two distinct transitions: an onset at 244 K associated with the cubic phase and a second near 220 K linked to the hexagonal phase. Notably, resistance profiles collected from multiple current and voltage permutations showed variations in transition width and onset temperature that correlated with the spatial phase distribution. These findings demonstrate a direct connection between local structural domains and superconducting behavior. 
    more » « less
  2. Abstract Recently, room temperature superconductivity was measured in a carbonaceous sulfur hydride material whose identity remains unknown. Herein, first-principles calculations are performed to provide a chemical basis for structural candidates derived by doping H3S with low levels of carbon. Pressure stabilizes unusual bonding configurations about the carbon atoms, which can be six-fold coordinated as CH6entities within the cubic H3S framework, or four-fold coordinated as methane intercalated into the H-S lattice, with or without an additional hydrogen in the framework. The doping breaks degenerate bands, lowering the density of states at the Fermi level (NF), and localizing electrons in C-H bonds. Low levels of CH4doping do not increaseNFto values as high as those calculated for$$Im\bar{3}m$$ I m 3 ¯ m -H3S, but they can yield a larger logarithmic average phonon frequency, and an electron–phonon coupling parameter comparable to that ofR3m-H3S. The implications of carbon doping on the superconducting properties are discussed. 
    more » « less
  3. The search for high-temperature superconductivity among pressure-stabilized hydrides has received great interest since theory-directed clathrate hydrides, such as CaH6, YH6, YH9, and LaH10, were synthesized and shown to exhibit a superconducting critical temperature (Tc) above 200 K. However, further tuning the superconductivity and stability of these prominent hydrides to enhance their applicability remains a significant challenge. Here, we take the sodalite-like clathrate prototype MH6 (M = Ca, Y, etc.) as an example to investigate the stability and superconductivity of multicomponent metal hydrides containing four different metal atoms for each structure. High-throughput simulations of 1820 ABCDH24 quinary hydrides with initial symmetry of F4" 3m, where A, B, C, and D represent different metal atoms were performed. The calculations reveal 119 structures that are dynamically stable at 300 GPa and 67 structures exhibit superconductivity exceeding 200 K, and 20 are found to have Tcs above 260 K. Notable among these quinary alloy hydrides, (Na,Zr,Mg,Hf)H6 is predicted to have a Tc approaching room temperature at 250 GPa. Both configurational and vibrational entropy play important roles in stabilizing these alloy structures. (Na,Y,Zr,Hf)H6, (Mg,Zr,Sc,Y)H6, and (Mg,Hf,Ca,Zr)H6 were computed to be thermodynamically stable, making them promising candidates for experimental synthesis. These quinary superconducting hydrides may facilitate realization of very high-temperature superconductors that are stable over a broader range of conditions than those found for binary or ternary systems. 
    more » « less
    Free, publicly-accessible full text available August 1, 2026
  4. Experimental constraints and sample limitations can preclude ideal measurements of electrical transport properties of materials. In such situations, AC electrical transport methods are often employed due to a significant increase in signal-to-noise ratio they can provide. However, dynamic effects that are not often accounted for may be present that may modify the signals in these measurements. In particular, dynamic filtering effects are prominent in small, granular, and heterogeneous materials. We demonstrate that a lock-in amplifier based circuit can distinguish between these DC transport and AC filtering effects. We further demonstrate that this filtering can reveal distinct signatures of magnetic transitions while providing a measure of sample quality. 
    more » « less
  5. In light of breakthroughs in superconductivity under high pressure, and considering that record critical temperatures (Tcs) across various systems have been achieved under high pressure, the primary challenge for higher Tcshould no longer solely be to increase Tcunder extreme conditions but also to reduce, or ideally eliminate, the need for applied pressure in retaining pressure-induced or -enhanced superconductivity. The topological semiconductor Bi0.5Sb1.5Te3(BST) was chosen to demonstrate our approach to addressing this challenge and exploring its intriguing physics. Under pressures up to ~50 GPa, three superconducting phases (BST-I, -II, and -III) were observed. A superconducting phase in BST-I appears at ~4 GPa, without a structural transition, suggesting the possible topological nature of this phase. Using the pressure-quench protocol (PQP) recently developed by us, we successfully retained this pressure-induced phase at ambient pressure and revealed the bulk nature of the state. Significantly, this demonstrates recovery of a pressure-quenched sample from a diamond anvil cell at room temperature with the pressure-induced phase retained at ambient pressure. Other superconducting phases were retained in BST-II and -III at ambient pressure and subjected to thermal and temporal stability testing. Superconductivity was also found in BST with Tcup to 10.2 K, the record for this compound series. While PQP maintains superconducting phases in BST at ambient pressure, both depressurization and PQP enhance its Tc, possibly due to microstructures formed during these processes, offering an added avenue to raise Tc. These findings are supported by our density-functional theory calculations. 
    more » « less
  6. The abrupt drop of resistance to zero at a critical temperature is a key signature of the current paradigm of the metal–superconductor transition. However, the emergence of an intermediate bosonic insulating state characterized by a resistance peak preceding the onset of the superconducting transition has challenged this traditional understanding. Notably, this phenomenon has been predominantly observed in disordered or chemically doped low-dimensional systems, raising intriguing questions about the generality of the effect and its underlying fundamental physics. Here, we present a systematic experimental study of compressed elemental sulfur, an undoped three-dimensional (3D) high-pressure superconductor, with detailed measurements of electrical resistance as a function of temperature, magnetic field, and current. The anomalous resistance peak observed in this 3D system is interpreted based on an empirical model of a metal–bosonic insulator–superconductor transition, potentially driven by vortex dynamics under magnetic field and energy dissipation processes. These findings offer a fresh platform for theoretical analysis of the decades-long enigmatic of the underlying mechanism of this phenomenon. 
    more » « less
  7. Recent band structure calculations have suggested the potential for band tuning in the chiral semiconductor Ag3AuTe2 to zero upon application of negative strain. In this study, we report on the synthesis of polycrystalline Ag3AuTe2 and investigate its transport and optical properties and mechanical compressibility. Transport measurements reveal the semiconducting behavior of Ag3AuTe2 with high resistivity and an activation energy Ea of 0.2 eV. The optical bandgap determined by diffuse reflectance measurements is about three times wider than the experimental Ea. Despite the difference, both experimental gaps fall within the range of predicted bandgaps by our first-principles density functional theory (DFT) calculations employing the Perdew–Burke–Ernzerhof and modified Becke–Johnson methods. Furthermore, our DFT simulations predict a progressive narrowing of the bandgap under compressive strain, with a full closure expected at a strain of −4% relative to the lattice parameter. To evaluate the feasibility of gap tunability at such substantial strain, the high-pressure behavior of Ag3AuTe2 was investigated by in situ high-pressure x-ray diffraction up to 47 GPa. Mechanical compression beyond 4% resulted in a pressure-induced structural transformation, indicating the possibility of substantial gap modulation under extreme compression conditions. 
    more » « less
  8. While hydrogen-rich materials have been demonstrated to exhibit high Tcsuperconductivity at high pressures, there is an ongoing search for ternary, quaternary, and more chemically complex hydrides that achieve such high critical temperatures at much lower pressures. First-principles searches are impeded by the computational complexity of solving the Eliashberg equations for large, complex crystal structures. Here, we adopt a simplified approach using electronic indicators previously established to be correlated with superconductivity in hydrides. This is used to study complex hydride structures, which are predicted to exhibit promisingly high critical temperatures for superconductivity. In particular, we propose three classes of hydrides inspired by the Fm 3 ¯ m RH 3 structures that exhibit strong hydrogen network connectivity, as defined through the electron localization function. The first class [RH 11 X 3 Y] is based on a Pm 3 ¯ m structure showing moderately high Tc, where the Tcestimate from electronic properties is compared with direct Eliashberg calculations and found to be surprisingly accurate. The second class of structures [(RH 11 ) 2 X 6 YZ] improves on this with promisingly high density of states with dominant hydrogen character at the Fermi energy, typically enhancing Tc. The third class [(R 1 H 11 )(R 2 H 11 )X 6 YZ] improves the strong hydrogen network connectivity by introducing anisotropy in the hydrogen network through a specific doping pattern. These design principles and associated model structures provide flexibility to optimize both Tcand the structural stability of complex hydrides. 
    more » « less