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1.
Adv Mater ; 33(15): e2006832, 2021 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-33751670

RESUMO

Pressure-stabilized hydrides are a new rapidly growing class of high-temperature superconductors, which is believed to be described within the conventional phonon-mediated mechanism of coupling. Here, the synthesis of one of the best-known high-TC superconductors-yttrium hexahydride I m 3 ¯ m -YH6 is reported, which displays a superconducting transition at ≈224 K at 166 GPa. The extrapolated upper critical magnetic field Bc2 (0) of YH6 is surprisingly high: 116-158 T, which is 2-2.5 times larger than the calculated value. A pronounced shift of TC in yttrium deuteride YD6 with the isotope coefficient 0.4 supports the phonon-assisted superconductivity. Current-voltage measurements show that the critical current IC and its density JC may exceed 1.75 A and 3500 A mm-2 at 4 K, respectively, which is higher than that of the commercial superconductors, such as NbTi and YBCO. The results of superconducting density functional theory (SCDFT) and anharmonic calculations, together with anomalously high critical magnetic field, suggest notable departures of the superconducting properties from the conventional Migdal-Eliashberg and Bardeen-Cooper-Schrieffer theories, and presence of an additional mechanism of superconductivity.

2.
J Phys Chem Lett ; 12(1): 32-40, 2021 Jan 14.
Artigo em Inglês | MEDLINE | ID: mdl-33296213

RESUMO

We conducted a joint experimental-theoretical investigation of the high-pressure chemistry of europium polyhydrides at pressures of 86-130 GPa. We discovered several novel magnetic Eu superhydrides stabilized by anharmonic effects: cubic EuH9, hexagonal EuH9, and an unexpected cubic (Pm3n) clathrate phase, Eu8H46. Monte Carlo simulations indicate that cubic EuH9 has antiferromagnetic ordering with TN of up to 24 K, whereas hexagonal EuH9 and Pm3n-Eu8H46 possess ferromagnetic ordering with TC = 137 and 336 K, respectively. The electron-phonon interaction is weak in all studied europium hydrides, and their magnetic ordering excludes s-wave superconductivity, except, perhaps, for distorted pseudohexagonal EuH9. The equations of state predicted within the DFT+U approach (U - J were found within linear response theory) are in close agreement with the experimental data. This work shows the great influence of the atomic radius on symmetry-breaking distortions of the crystal structures of superhydrides and on their thermodynamic stability.

3.
Molecules ; 25(17)2020 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-32825707

RESUMO

Recently, the iron containing langasite-type crystal Ba3NbFe3Si2O14 has attracted great attention as a new magnetically induced multiferroic. In this work, magnetic, structural and electronic properties of the multiferroic Ba3NbFe3Si2O14 were investigated by several methods, including synchrotron X-ray diffraction, Raman spectroscopy and synchrotron Mössbauer source technique at high quasi-hydrostatic pressures (up to 70 GPa), created in diamond anvil cells. At room temperature, two structural transitions at pressures of about 3.0 and 17.5 GPa were detected. Mössbauer studies at high pressures revealed a radical change in the magnetic properties during structural transitions. At pressures above 18 GPa, the crystal transforms into two magnetic fractions, and in one of them the Néel temperature (TN) increases by about four times compared with the TN value in the initial phase (from 27 to 115 K). At pressures above 50 GPa, a spin crossover occurs when the fraction of iron Fe3+ ions in oxygen octahedra transits from the high-spin (HS, S = 5/2) to the low-spin (LS, S = 1/2) state. This leads to a new change in the magnetic properties. The magnetic ordering temperature of the LS sublattice was found to be of about 22(1) K, and magnetic correlations between HS and LS sublattices were studied.


Assuntos
Bário/química , Compostos Férricos/química , Magnetismo , Nióbio/química , Silicatos/química , Marcadores de Spin , Cristalografia por Raios X , Pressão , Espectroscopia de Mossbauer , Análise Espectral Raman , Difração de Raios X
4.
Science ; 351(6279): 1303-6, 2016 Mar 18.
Artigo em Inglês | MEDLINE | ID: mdl-26989248

RESUMO

High-temperature superconductivity remains a focus of experimental and theoretical research. Hydrogen sulfide (H2S) has been reported to be superconducting at high pressures and with a high transition temperature. We report on the direct observation of the expulsion of the magnetic field in H2S compressed to 153 gigapascals. A thin (119)Sn film placed inside the H2S sample was used as a sensor of the magnetic field. The magnetic field on the (119)Sn sensor was monitored by nuclear resonance scattering of synchrotron radiation. Our results demonstrate that an external static magnetic field of about 0.7 tesla is expelled from the volume of (119)Sn foil as a result of the shielding by the H2S sample at temperatures between 4.7 K and approximately 140 K, revealing a superconducting state of H2S.

5.
Proc Natl Acad Sci U S A ; 110(18): 7142-7, 2013 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-23589892

RESUMO

Ferropericlase [(Mg,Fe)O] is one of the most abundant minerals of the earth's lower mantle. The high-spin (HS) to low-spin (LS) transition in the Fe(2+) ions may dramatically alter the physical and chemical properties of (Mg,Fe)O in the deep mantle. To understand the effects of compression on the ground electronic state of iron, electronic and magnetic states of Fe(2+) in (Mg0.75Fe0.25)O have been investigated using transmission and synchrotron Mössbauer spectroscopy at high pressures and low temperatures (down to 5 K). Our results show that the ground electronic state of Fe(2+) at the critical pressure Pc of the spin transition close to T = 0 is governed by a quantum critical point (T = 0, P = P(c)) at which the energy required for the fluctuation between HS and LS states is zero. Analysis of the data gives P(c) = 55 GPa. Thermal excitation within the HS or LS states (T > 0 K) is expected to strongly influence the magnetic as well as physical properties of ferropericlase. Multielectron theoretical calculations show that the existence of the quantum critical point at temperatures approaching zero affects not only physical properties of ferropericlase at low temperatures but also its properties at P-T of the earth's lower mantle.

6.
Phys Rev Lett ; 109(8): 086402, 2012 Aug 24.
Artigo em Inglês | MEDLINE | ID: mdl-23002762

RESUMO

The insulator-metal transition was observed experimentally in nickel monoxide (NiO) at very high pressures of ~240 GPa. The sample resistance becomes measurable at about 130 GPa and decreases substantially with the pressure increase to ~240 GPa. A sharp drop in resistance by about 3 orders of magnitude has been observed at ~240 GPa with a concomitant change of the resistance type from semiconducting to metallic. This is the first experimental observation of an insulator-metal transition in NiO, which was anticipated by Mott decades ago. From simple multielectron consideration, the metallic phase of NiO forms when the effective Hubbard energy U(eff) is almost equal to the estimated full bandwidth 2W.

7.
Nat Mater ; 3(8): 558-63, 2004 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-15235595

RESUMO

Nitrogen usually consists of molecules where two atoms are strongly triple-bonded. Here, we report on an allotropic form of nitrogen where all atoms are connected with single covalent bonds, similar to carbon atoms in diamond. The compound was synthesized directly from molecular nitrogen at temperatures above 2,000 K and pressures above 110 GPa using a laser-heated diamond cell. From X-ray and Raman scattering we have identified this as the long-sought-after polymeric nitrogen with the theoretically predicted cubic gauche structure (cg-N). This cubic phase has not been observed previously in any element. The phase is a stiff substance with bulk modulus >or=300 GPa, characteristic of strong covalent solids. The polymeric nitrogen is metastable, and contrasts with previously reported amorphous non-molecular nitrogen, which is most likely a mixture of small clusters of non-molecular phases. The cg-N represents a new class of single-bonded nitrogen materials with unique properties such as energy capacity: more than five times that of the most powerfully energetic materials.


Assuntos
Cristalização/métodos , Manufaturas , Nanotecnologia/métodos , Nitrogênio/química , Cristalografia , Teste de Materiais , Conformação Molecular , Transição de Fase , Pressão , Temperatura
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