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A fascinating feature of metallic glasses is their ability to explore different configurations under mechanical deformations. This effect is usually observed through macroscopic observables, while little is known on the consequence of the deformation at atomic level. Using the new generation of synchrotrons, we probe the atomic motion and structure in a metallic glass under hydrostatic compression, from the onset of the perturbation up to a severely-compressed state. While the structure indicates reversible densification under compression, the dynamic is dramatically accelerated and exhibits a hysteresis with two regimes. At low pressures, the atomic motion is heterogeneous with avalanche-like rearrangements suggesting rejuvenation, while under further compression, aging leads to a super-diffusive dynamics triggered by internal stresses inherent to the glass. These results highlight the complexity of the atomic motion in non-ergodic systems and support a theory recently developed to describe the surprising rejuvenation and strain hardening of metallic glasses under compression., Comment: 16 pages, 5 figures + Supplementary Information (7 pages, 9 figures). First submitted version of manuscript

Doped IrTe$_2$ is considered a platform for topological superconductivity and therefore receives currently a lot of interest. In addition, the superconductivity in these materials exists in close vicinity of electronic valence bond crystals, which we explore here by means of high-pressure single crystal x-ray diffraction in combination with density functional theory. Our crystallographic refinements provide unprecedented information about the structural evolution as a function of applied pressure up to 42 GPa. Using this structural information for density functional theory calculations, we show that the valence bond formation in IrTe$_2$ is driven by changes in the Ir-Te-Ir bond angle. When a valence bond is formed, this bond angle decreases drastically, leading to a stabilization of local valence bonds large enough to push them out of a broad band continuum. This unusual local mechanism of valence bond formation in an itinerant material provides a natural explanation for the different valence bond orders in IrTe$_2$, implies a very strong electron-phonon coupling and is most likely relevant for the superconductivity as well., Comment: 10 pages, 6 figures

Cubic Pm-3n Nb3Sn0.92 superconductor (Tc ~ 16 K) was found to exhibit tetragonal instabilities at the superconducting state (T = 10 K). These instabilities are manifested through the appearance of reflections which are forbidden in the Pm-3n symmetry but are compatible with the P42/mmc structure which is observed in the Nb3Sn1-x system for higher Sn content at temperatures lower than ~ 43 K. Nevertheless, the low-temperature structure of Nb3Sn0.92 remains metrically fully cubic, as concluded from single crystal synchrotron radiation diffraction experiments. Subsequent application of external pressure amplifies the observed instabilities with a resulting pseudo-cubic - tetragonal transformation at P = 3 GPa at 10 K and this transition is energy driven, as concluded from ab initio calculations. The electronic structures of the corresponding phases are virtually identical and, therefore, the pseudo-cubic - tetragonal transformation does not influence significantly the underlying electronic interactions. Consequently, no anomalies in the behavior of the critical temperature, Tc, are expected at this pressure. However, anomalies in the upper critical field are anticipated during this transition, in analogy to the corresponding behavior observed during the cubic-tetragonal transformation in Nb3Sn1-x induced by increase in Sn content. Therefore targeted changes in composition could be used to enhance upper critical field of Nb3Sn1-x for specific extreme conditions of temperature and pressure.

Application of high pressure (HP) induces evolution from metallic to semi-metallic state in the layered superconducting LaO1-xFxBiSe2 phase, as concluded from ab initio calculations based on experimental P-dependent structural data. These changes in conduction properties are associated with a reported decrease in the superconducting transition temperature, Tc. However, further increase in pressure induces structural transformation in LaO1-xFxBiSe2 which results in a strong enhancement of its two-dimensionality with a related improvement in superconducting performance. In addition, the HP structural anisotropy induces a loss of long-range order correlations along the stacking direction of the LaO/F and BiSe2 layers yielding formation of stacking faults. Similar but even more pronounced structural transition was observed in the related LaO1-xFxBiS2 phase which is also accompanied by an increase in Tc. This demonstrates that enhancement of two-dimensionality in layered superconducting systems acts in favor of their superconducting performance.

We report a combined experimental and theoretical study of the melting curve and the structural behavior of vanadium under extreme pressure and temperature. We performed powder x-ray diffraction experiments up to 120 GPa and 4000 K, determining the phase boundary of the bcc-to-rhombohedral transition and melting temperatures at different pressures. Melting temperatures have also been established from the observation of temperature plateaus during laser heating, and the results from the density-functional theory calculations. Results obtained from our experiments and calculations are fully consistent and lead to an accurate determination of the melting curve of vanadium. These results are discussed in comparison with previous studies. The melting temperatures determined in this study are higher than those previously obtained using the speckle method, but also considerably lower than those obtained from shock-wave experiments and linear muffin-tin orbital calculations. Finally, a high-pressure high-temperature equation of state up to 120 GPa and 2800 K has also been determined., Comment: 20 pages, 5 figures

This work reports on the pressure dependence of the octahedra tilts and mean Fe-O bond lengths in RFeO3 (R=Nd, Sm, Eu, Gd, Tb and Dy), determined through synchrotron X-ray diffraction and Raman scattering, and their role on the pressure induced phase transition displayed by all of these compounds. For larger rare-earth cations (Nd-Sm), both anti- and in-phase octahedra tilting decrease as pressure increases, whereas the reverse behavior is observed for smaller ones (Gd-Dy). EuFeO3 stands at the borderline, as the tilts are pressure independent. For the compounds where the tilts increase with pressure, the FeO6 octahedra are compressed at lower rates than for those ones exhibiting opposite pressure tilt dependence. The crossover between the two opposite pressure behaviors is discussed and faced with the rules grounded on the current theoretical approaches. The similarity of the pressure-induced isostructural insulator-to-metal phase transition, observed in the whole series, point out that the tilts play a minor role in its driving mechanisms. A clear relationship between octahedra compressibility and critical pressure is ascertained., Comment: 25 pages (including Supplemental Information), 12 figures and 4 tables

There is a direct relation between the composition of a host star and that of the planets orbiting around it. As such, the recent discovery of stars with unusual chemical composition, notably enriched in carbon instead of oxygen, support the existence of exoplanets with a chemistry dominated by carbides instead of oxides. Accordingly several studies have been recently conducted on the Si C binary system at high pressure and temperature. Nonetheless, the properties of carbides at the P T conditions of exoplanets interiors are still inadequately constrained, effectively hampering reliable planetary modeling. Here we present an in situ X ray diffraction study of the Si C binary system up to 200 GPa and 3500 K, significantly enlarging the pressure range explored by previous experimental studies. The large amount of collected data allows us to properly investigate the phase diagram and to refine the Clapeyron slope of the transition line from the zinc blende to the rock salt structure. Furthermore the pressure volume temperature equation of state are provided for the high pressure phase, characterized by low compressibility and thermal expansion. Our results are used to model idealized C rich exoplanets of end members composition. In particular, we derived mass radius relations and performed numerical simulations defining rheological parameters and initial conditions which lead to onset of convection in such SiC planets. We demonstrate that if restrained to silicate rich mantle compositions, the interpretation of mass radius relations may underestimate the interior diversity of exoplanets., Comment: 30 Pages, 8 Figures

BaFe2Se3 is a potential superconductor material exhibiting transition at 11 K and ambient pressure. Here we extended the structural and performed electrical resistivity measurements on this compound up to 51 GPa and 20 GPa, respectively, in order to distinguish if the superconductivity in this sample is intrinsic to the BaFe2Se3 phase or if it is originating from minor FeSe impurities that show a similar superconductive transition temperature. The electrical resistance measurements as a function of pressure show that at 5 GPa the superconducting transition is observed at around 10 K, similar to the one previously observed for this sample at ambient pressure. This indicates that the superconductivity in this sample is intrinsic to the BaFe2Se3 phase and not to FeSe with Tc > 20 K at these pressures. Further increase in pressure suppressed the superconductive signal and the sample remained in an insulating state up to the maximum achieved pressure of 20 GPa. Single-crystal and powder X-ray diffraction measurements revealed two structural transformations in BaFe2Se3: a second order transition above 3.5 GPa from Pnma (CsAg2I3-type structure) to Cmcm (CsCu2Cl3-type structure) and a first order transformation at 16.6 GPa. Here, {\gamma}-BaFe2Se3 transforms into {\delta}-BaFe2Se3 (Cmcm, CsCu2Cl3-type average structure) via a first order phase transition mechanism. This transitions is characterized by a significant shortening of the b lattice parameter of {\gamma}-BaFe2Se3 (17%) and accompanied by an anisotropic expansion in the orthogonal ac plane at the transition point.

A single-phase high pressure (HP) modification of CsxFe2-ySe2 was synthesized at 11.8 GPa at ambient temperature. Structurally this polymorph is similar to the minor low pressure (LP) superconducting phase, namely they both crystallize in a ThCr2Si2-type structure without ordering of the Fe vacancies within the Fe-deficient FeSe4 layers. The HP CsxFe2-ySe2 polymorph is found to be less crystalline and nearly twice as soft compared to the parent major and minor phases of CsxFe2-ySe2. It can be quenched to low pressures and is stable at least on the scale of weeks. At ambient pressure the HP polymorph of CsxFe2-ySe2 is expected to exhibit different superconducting properties compared to its LP minor phase (Tc = 27 K).

Single crystal synchrotron X-ray diffraction as a function of temperature and pressure has revealed a complex biphase mixture in superconducting FeSe. Based on our experimental results we construct a phase diagram where structural behavior and superconducting properties of FeSe are found to be correlated. We show that below 6 GPa, where pressure promotes the superconducting critical temperature, the FeSe structure is composed of 2D layers of edge-shared FeSe4 tetrahedra, while above 6 GPa the superconductivity is strongly suppressed on formation of a new orthorhombic polymorph characterized by a 3D network of face sharing FeSe6 octahedra. Therefore changes in topology and connectivity of the FeSe structure are found to be detrimental for superconductivity to exist. This previously controversial crystal structure of the high pressure polymorph of FeSe was also unambiguously determined. High pressure FeSe adopts an orthorhombic MnP-type structure (Pnma) which corresponds to a slightly distorted hexagonal NiAs-type arrangement (P63/mmc). The structural transformation from the low- to high-pressure FeSe polymorph is first order in nature and is manifested as antiparallel displacements within the Fe and Se sublattices.

The structural transformation of multiferroic EuTiO$_3$ has been intensively investigated by synchrotron x-ray diffraction at pressures up to 50.3 GPa and temperatures from 50 to 500 K. An antiferrodistortive phase transition from cubic Pm-3m to tetragonal I4/mcm space group has been observed, identical to the one that has been previously explored at ambient pressure and low temperatures. Several compression/decompression cycles at different temperatures have been carried out to accurately map the transition, and as a result a P-T phase diagram for EuTiO$_3$ has been constructed. The observed phase transition exhibits many similarities with isostructural SrTiO$_3$, although the absence of magnetoelectric interactions in the latter accounts for the different phase boundaries between the two materials.

Pressure-dependent diffraction response of the superconducting phase separated Cs0.72Fe1.57Se2 has been studied using synchrotron radiation up to the pressure of 19 GPa. The main and secondary phases of Cs0.72Fe1.57Se2 have been observed in the whole pressure range. The main ordered phase has been found to undergo an order-disorder transition in the Fe-sublattice at least at P = 11 GPa with the corresponding kinetics on the order of hours. Contrary to the analogous temperature induced transition, the secondary phase has not been suppressed suggesting that its stability pressure range is higher than 19 GPa or the corresponding transformation kinetics is slower at room temperature. Together with the previously reported pressure-dependent resistivity and magnetic susceptibility measurements, this work indicates that superconductivity in the AxFe2-ySe2 (A - alkali metals) phases could be related to the Fe-vacancy ordering in the main phase.

We report experimental and theoretical evidence that solid molecular ammonia becomes unstable at room temperature and high pressures and transforms into an ionic crystalline form. This material has been characterised in both hydrogenated NH3 and deuterated ND3 ammonia samples up to about 180 and 200 GPa, respectively, by infrared absorption, Raman spectroscopy and x-ray diffraction. The presence of a new, strong IR absorption band centered at 2500 cm-1 in NH3 (1900 cm-1 in ND3) signals the ionization of ammonia molecules into NH2- and NH4+ ions, in line with previous theoretical predictions. We find experimental evidence for a coexistence of two crystalline ionic forms, which our ab-initio structure searches predict to be the most stable at the relevant pressures. The ionic crystalline form of ammonia is stable at low temperatures, which contrasts with the behaviour of water in which no equivalent crystalline ionic phase has been found., Comment: 7 pages, 7 figures

Compressibility of high-purity nanostructured cBN has been studied under quasi-hydrostatic conditions at 300 K up to 35 GPa using diamond anvil cell and angle-dispersive synchrotron X-ray powder diffraction. A data fit to the Vinet equation of state yields the values of the bulk modulus B0 of 375(4) GPa with its first pressure derivative B0' of 2.3(3). The nanometer grain size (\sim20 nm) results in decrease of the bulk modulus by ~9%.

The electrical resistivity, crystalline structure and electronic properties calculated from the experimentally measured atomic positions of the compound SmFeAsO$_{0.81}$F$_{0.19}$ have been studied up to pressures ~20GPa. The correlation between the pressure dependence of the superconducting transition temperature (Tc) and crystallographic parameters on the same sample shows clearly that a regular FeAs$_{4}$ tetrahedron maximizes Tc, through optimization of carrier transfer to the FeAs planes as indicated by the evolution of the electronic band structures., Comment: 15pages, 4 figures

We have studied the structural and superconducting properties of tetragonal FeSe under pressures up to 26GPa using synchrotron radiation and diamond anvil cells. The bulk modulus of the tetragonal phase is 28.5(3)GPa, much smaller than the rest of Fe based superconductors. At 12GPa we observe a phase transition from the tetragonal to an orthorhombic symmetry. The high pressure orthorhombic phase has a higher Tc reaching 34K at 22GPa., Comment: 15 pages, 4 figures

We have studied the structural and superconductivity properties of the compound LaFeAsO0.9F0.1 under pressures up to 32GPa using synchrotron radiation and diamond anvil cells. We obtain an ambient pressure bulk modulus K_0 = 78(2)GPa, compressibility comparable to some cuprates. At high pressures, the sample is in the overdoped region, with a linear decrease with pressure variation of the superconducting transition temperature., Comment: 15 pages, 4 figures, 1 table

The pressure effects on the JT distortion of three representative compounds belonging to the LaMn_1-xGa_xO_3 (x= 0.2, 0.3, 0.4) family was widely investigated by means of X-ray diffraction and Raman spectroscopy. A compound with a fully JT distorted structure (x=0.2), one with regular octahedra (x=0.6) and one in an intermediate configuration (x=0.3) were selected. A pressure induced transitions from the orthorhombic Pbnm phase towards structures with higher symmetry were observed in all the samples. Both Raman and X-ray data confirm that the most important structural effect of pressure is that of reducing the octahedral distortion. The appearance of a feature in the lattice parameter behavior connected to a structural instability was also detected, pointing out the key role of the JT distortion in stabilizing the manganite structures. On the other hand, the complete suppression of the JT distortion in the high-pressure phases cannot be claimed. The Raman spectra collected from more distorted compounds (x=0.2, 0.3) reveal clearly the coexistence of domains of distorted and more regular octahedra in a certain pressure range. The first sketch of the Pressure vs. Ga-content phase diagram was drawn., Comment: LateX v2.6, 9 pages with 10 figures

By means of synchrotron X-ray diffraction, we studied the effect of high pressure, P, up to 13 GPa on the room temperature crystal structure of superconducting CaC6. In this P range, no change of the pristine space group symmetry, \textit{R\=3m}, is found. However, at 9 GPa, i.e. close to the critical value at which a large T_c reduction was reported recently, we observed a compressibility jump concomitant to a large broadening of Bragg peaks. The reversibility of both effects upon depressurization and symmetry arguments give evidence of an order-disorder phase transition of second order, presumably associated with the Ca sublattice, which provides a full account for the above Tc reduction., Comment: 9 pages, 3 figures

The high pressure phase diagram of CsC8 graphite intercalated compound has been investigated at ambient temperature up to 32 GPa. Combining X-ray and neutron diffraction, Raman and X- ray absorption spectroscopies, we report for the first time that CsC8, when pressurized, undergoes phase transitions around 2.0, 4.8 and 8 GPa. Possible candidate lattice structures and the transition mechanism involved are proposed. We show that the observed transitions involve the structural re- arrangement in the Cs sub-network while the distance between the graphitic layers is continuously reduced at least up to 8.9 GPa. Around 8 GPa, important modifications of signatures of the electronic structure measured by Raman and X-ray absorption spectroscopies evidence the onset of a new transition.

The low-lying magnetic excitations in the dimer of single-molecule magnets (Mn4)2 are studied by inelastic neutron scattering as a function of hydrostatic pressure. The anisotropy parameters D and B04, which describe each Mn4 subunit, are essentially pressure independent, while the antiferromagnetic exchange coupling J between the two Mn4 subunits strongly depends on pressure, with an increase of 42% at 17 kbar. Additional pressure dependent powder X-ray measurements allow a structural interpretation of the findings., Comment: 4 pages, 4 figures, REVTEX4, to be published in PRB

We report measurements on MgB2 up to ~40GPa. Increasing pressure yields a monotonous decrease of the lattice parameters and of the c/a ratio, but no structural transition down to parameters smaller than those of AlB2. The transition superconducting temperature also decreases with temperature in a sample dependent way. The results are explained by an increase of the filling of the 2D pxy bands with pressure, the Mg stoichiometry determining the starting position of the Fermi level. Our measurements indicate that these hole bands are the relevant ones for superconductivity., Comment: submitted March 9th 2001, PRB accepted