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2.
Chem Commun (Camb) ; 60(8): 1047, 2024 Jan 23.
Article in English | MEDLINE | ID: mdl-38223922

ABSTRACT

Retraction of 'Carbon content drives high temperature superconductivity in a carbonaceous sulfur hydride below 100 GPa' by G. Alexander Smith et al., Chem. Commun., 2022, 58, 9064-9067, https://doi.org/10.1039/D2CC03170A.

6.
Nature ; 615(7951): 244-250, 2023 03.
Article in English | MEDLINE | ID: mdl-36890373

ABSTRACT

The absence of electrical resistance exhibited by superconducting materials would have enormous potential for applications if it existed at ambient temperature and pressure conditions. Despite decades of intense research efforts, such a state has yet to be realized1,2. At ambient pressures, cuprates are the material class exhibiting superconductivity to the highest critical superconducting transition temperatures (Tc), up to about 133 K (refs. 3-5). Over the past decade, high-pressure 'chemical precompression'6,7 of hydrogen-dominant alloys has led the search for high-temperature superconductivity, with demonstrated Tc approaching the freezing point of water in binary hydrides at megabar pressures8-13. Ternary hydrogen-rich compounds, such as carbonaceous sulfur hydride, offer an even larger chemical space to potentially improve the properties of superconducting hydrides14-21. Here we report evidence of superconductivity on a nitrogen-doped lutetium hydride with a maximum Tc of 294 K at 10 kbar, that is, superconductivity at room temperature and near-ambient pressures. The compound was synthesized under high-pressure high-temperature conditions and then-after full recoverability-its material and superconducting properties were examined along compression pathways. These include temperature-dependent resistance with and without an applied magnetic field, the magnetization (M) versus magnetic field (H) curve, a.c. and d.c. magnetic susceptibility, as well as heat-capacity measurements. X-ray diffraction (XRD), energy-dispersive X-ray (EDX) and theoretical simulations provide some insight into the stoichiometry of the synthesized material. Nevertheless, further experiments and simulations are needed to determine the exact stoichiometry of hydrogen and nitrogen, and their respective atomistic positions, in a greater effort to further understand the superconducting state of the material.

8.
Chem Commun (Camb) ; 58(65): 9064-9067, 2022 Aug 11.
Article in English | MEDLINE | ID: mdl-35837875

ABSTRACT

We report a previously unobserved superconducting state of the photosynthesized carbonaceous sulfur hydride (C-S-H) system with a maximum TC of 191(1) K below 100 GPa. The properties of C-S-H are dependent on carbon content, and X-ray diffraction and simulations reveal the system remains molecular-like up to 100 GPa.

9.
J Chem Phys ; 155(11): 114703, 2021 Sep 21.
Article in English | MEDLINE | ID: mdl-34551552

ABSTRACT

X-ray diffraction indicates that the structure of the recently discovered carbonaceous sulfur hydride (C-S-H) room-temperature superconductor is derived from previously established van der Waals compounds found in the H2S-H2 and CH4-H2 systems. Crystals of the superconducting phase were produced by a photochemical synthesis technique, leading to the superconducting critical temperature Tc of 288 K at 267 GPa. X-ray diffraction patterns measured from 124 to 178 GPa, within the pressure range of the superconducting phase, are consistent with an orthorhombic structure derived from the Al2Cu-type determined for (H2S)2H2 and (CH4)2H2 that differs from those predicted and observed for the S-H system at these pressures. The formation and stability of the C-S-H compound can be understood in terms of the close similarity in effective volumes of the H2S and CH4 components, and denser carbon-bearing S-H phases may form at higher pressures. The results are crucial for understanding the very high superconducting Tc found in the C-S-H system at megabar pressures.

10.
Adv Mater ; 33(39): e2103000, 2021 Oct.
Article in English | MEDLINE | ID: mdl-34397123

ABSTRACT

The competing and non-equilibrium phase transitions, involving dynamic tunability of cooperative electronic and magnetic states in strongly correlated materials, show great promise in quantum sensing and information technology. To date, the stabilization of transient states is still in the preliminary stage, particularly with respect to molecular electronic solids. Here, a dynamic and cooperative phase in potassium-7,7,8,8-tetracyanoquinodimethane (K-TCNQ) with the control of pulsed electromagnetic excitation is demonstrated. Simultaneous dynamic and coherent lattice perturbation with 8 ns pulsed laser (532 nm, 15 MW cm-2 , 10 Hz) in such a molecular electronic crystal initiates a stable long-lived (over 400 days) conducting paramagnetic state (≈42 Ωcm), showing the charge-spin bistability over a broad temperature range from 2 to 360 K. Comprehensive noise spectroscopy, in situ high-pressure measurements, electron spin resonance (ESR), theoretical model, and scanning tunneling microscopy/spectroscopy (STM/STS) studies provide further evidence that such a transition is cooperative, requiring a dedicated charge-spin-lattice decoupling to activate and subsequently stabilize nonequilibrium phase. The cooperativity triggered by ultrahigh-strain-rate (above 106 s- 1 ) pulsed excitation offers a collective control toward the generation and stabilization of strongly correlated electronic and magnetic orders in molecular electronic solids and offers unique electro-magnetic phases with technological promises.

11.
Phys Rev Lett ; 127(1): 016401, 2021 Jul 02.
Article in English | MEDLINE | ID: mdl-34270285

ABSTRACT

A reversible density driven insulator to metal to insulator transition in high-spin MnS_{2} is experimentally observed, leading with a colossal electrical resistance drop of 10^{8} Ω by 12 GPa. Density functional theory simulations reveal the metallization to be unexpectedly driven by previously unoccupied S_{2}^{2-} σ_{3p}^{*} antibonding states crossing the Fermi level. This is a unique variant of the charge transfer insulator to metal transition for negative charge transfer insulators having anions with an unsaturated valence. By 36 GPa the emergence of the low-spin insulating arsenopyrite (P2_{1}/c) is confirmed, and the bulk metallicity is broken with the system returning to an insulative electronic state.

12.
Phys Rev Lett ; 126(11): 117003, 2021 Mar 19.
Article in English | MEDLINE | ID: mdl-33798352

ABSTRACT

The recent observation of room-temperature superconductivity will undoubtedly lead to a surge in the discovery of new, dense, hydrogen-rich materials. The rare earth metal superhydrides are predicted to have very high-T_{c} superconductivity that is tunable with changes in stoichiometry or doping. Here we report the synthesis of an yttrium superhydride that exhibits superconductivity at a critical temperature of 262 K at 182±8 GPa. A palladium thin film assists the synthesis by protecting the sputtered yttrium from oxidation and promoting subsequent hydrogenation. Phonon-mediated superconductivity is established by the observation of zero resistance, an isotope effect and the reduction of T_{c} under an external magnetic field. The upper critical magnetic field is 103 T at zero temperature.

13.
Nature ; 588(7837): E18, 2020 Dec.
Article in English | MEDLINE | ID: mdl-33214713

ABSTRACT

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

14.
Nature ; 586(7829): 373-377, 2020 10.
Article in English | MEDLINE | ID: mdl-33057222

ABSTRACT

One of the long-standing challenges in experimental physics is the observation of room-temperature superconductivity1,2. Recently, high-temperature conventional superconductivity in hydrogen-rich materials has been reported in several systems under high pressure3-5. An  important discovery leading to room-temperature superconductivity is the pressure-driven disproportionation of hydrogen sulfide (H2S) to H3S, with a confirmed transition temperature of 203 kelvin at 155 gigapascals3,6. Both H2S and CH4 readily mix with hydrogen to form guest-host structures at lower pressures7, and are of  comparable size at 4 gigapascals. By introducing methane at low pressures into the H2S + H2 precursor mixture for H3S, molecular exchange is allowed within a large assemblage of van der Waals solids that are hydrogen-rich with H2 inclusions; these guest-host structures become the building blocks of superconducting compounds at extreme conditions. Here we report superconductivity in a photochemically transformed carbonaceous sulfur hydride system, starting from elemental precursors, with a maximum superconducting transition temperature of 287.7 ± 1.2 kelvin (about 15 degrees Celsius) achieved at 267 ± 10 gigapascals. The superconducting state is observed over a broad pressure range in the diamond anvil cell, from 140 to 275 gigapascals, with a sharp upturn in transition temperature above 220 gigapascals. Superconductivity is established by the observation of zero resistance, a magnetic susceptibility of up to 190 gigapascals, and reduction of the transition temperature under an external magnetic field of up to 9 tesla, with an upper critical magnetic field of about 62 tesla according to the Ginzburg-Landau model at zero temperature. The light, quantum nature of hydrogen limits the structural and stoichiometric determination of the system by X-ray scattering techniques, but Raman spectroscopy is used to probe the chemical and structural transformations before metallization. The introduction of chemical tuning within our ternary system could enable the preservation of the properties of room-temperature superconductivity at lower pressures.

15.
J Phys Chem Lett ; 10(18): 5351-5356, 2019 Sep 19.
Article in English | MEDLINE | ID: mdl-31436423

ABSTRACT

Many rutile-type materials are characterized by a softness in shear with pressure which is coupled to a Raman-active librational motion. Combining direct studies of anion positions in SnO2 with measurements of its electronic properties, we find a correlation between O sublattice disorder between 5 and 10 GPa and an anomalous decrease up to 4 orders of magnitude in electrical resistance. Hypotheses into the atomistic nature of the phenomenon are evaluated via ab initio calculations guided by extended X-ray absorption fine structure spectroscopy analysis, and the most likely mechanism is found to be the displacement of single anions resulting from the pressure-induced softening of the librational mode. On the basis of this mechanism, we propose that the same behavior should feature across all materials exhibiting a rutile → CaCl2 phase transition and that conductivity in other rutile-type materials could be facilitated at ambient pressure by appropriate design of devices to enhance defects of this nature.

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