The Extreme Conditions Beamline P02.2 and the Extreme Conditions Science Infrastructure at PETRA III.

A detailed description is presented of the Extreme Conditions Beamline P02.2 for micro X-ray diffraction studies of matter at simultaneous high pressure and high/low temperatures at PETRA III, in Hamburg, Germany. This includes performance of the X-ray optics and instrumental resolution as well as an overview of the different sample environments available for high-pressure studies in the diamond anvil cell. Particularly emphasized are the high-brilliance and high-energy X-ray diffraction capabilities of the beamline in conjunction with the use of fast area detectors to conduct time-resolved compression studies in the millisecond time regime. Finally, the current capability of the Extreme Conditions Science Infrastructure to support high-pressure research at the Extreme Conditions Beamline and other PETRA III beamlines is described.

The surface modification of the silica-coated magnetic nanoparticles and their application in molecular diagnostics of virus infection.

The study presents a series of examples of magnetic nanoparticle systems designed for the diagnosis of viral diseases. In this interdisciplinary work, we describe one of the most comprehensive synthetic approaches for the preparation and functionalization of smart nanoparticle systems for rapid and effective RT-PCR diagnostics and isolation of viral RNA. Twelve different organic ligands and inorganic porous silica were used for surface functionalization of the Fe3O4 magnetic core to increase the number of active centres for efficient RNA binding from human swab samples. Different nanoparticle systems with common beads were characterized by HRTEM, SEM, FT-IR, XRD, XPS and magnetic measurements. We demonstrate the application of the fundamental models modified to fit the experimental zero-field cooling magnetization data. We discuss the influence of the nanoparticle shell parameters (morphology, thickness, ligands) on the overall magnetic performance of the systems. The prepared nanoparticles were tested for the isolation of viral RNA from tissue samples infected with hepatitis E virus-HEV and from biofluid samples of SARS-CoV-2 positive patients. The efficiency of RNA isolation was quantified by RT-qPCR method.

A resistively-heated dynamic diamond anvil cell (RHdDAC) for fast compression x-ray diffraction experiments at high temperatures.

A resistively-heated dynamic diamond anvil cell (RHdDAC) setup is presented. The setup enables the dynamic compression of samples at high temperatures by employing a piezoelectric actuator for pressure control and internal heaters for high temperature. The RHdDAC facilitates the precise control of compression rates and was tested in compression experiments at temperatures up to 1400 K and pressures of ∼130 GPa. The mechanical stability of metallic glass gaskets composed of a FeSiB alloy was examined under simultaneous high-pressure/high-temperature conditions. High-temperature dynamic compression experiments on H2O ice and (Mg, Fe)O ferropericlase were performed in combination with time-resolved x-ray diffraction measurements to characterize crystal structures and compression behaviors. The employment of high brilliance synchrotron radiation combined with two fast GaAs LAMBDA detectors available at the Extreme Conditions Beamline (P02.2) at PETRA III (DESY) facilitates the collection of data with excellent pressure resolution. The pressure-temperature conditions achievable with the RHdDAC combined with its ability to cover a wide range of compression rates and perform tailored compression paths offers perspectives for a variety of future experiments under extreme conditions.

Fe2O3 and Gd2O3 nanoparticles loaded in mesoporous silica: insights into influence of NPs concentration and silica dimensionality.

Fine Fe2O3 and Gd2O3 magnetic nanoparticles (NPs) with sizes 7 nm and 10 nm embedded into mesoporous silica have been prepared using a wet-impregnation method. A comparative study of the reactant concentration along with the hosting matrix symmetry on mesostructuring and the magnetic properties of the nanocomposites have been investigated. Reactants with four different concentrations of Fe3+ and Gd3+ ions and silica matrices with two different kinds of symmetry (hexagonal and cubic) have been utilized for the study. The structural characterization of the samples has been carried out by the N2 adsorption/desorption method, high-energy X-ray diffraction (HE-XRD), TG/DTA, and high resolution transmission electron microscopy (HRTEM). The magnetic properties of the nanocomposites have been examined by means of SQUID magnetometry. It has been found that a range of different magnetic states (diamagnetic, paramagnetic, ferromagnetic, superparamagnetic) can be induced by the feasible tailoring of the particle concentration, the porous matrix symmetry and the composition. Furthermore, the existence of a "critical concentration limit" for embedding the particles within the body of the matrix has been confirmed. Exceeding the limit results in the expulsion of nanoparticles on the outer surface of the mesoporous matrix. Revelation of the relationships between particle concentration, matrix symmetry and magnetic properties of the particular composite reported in this study may facilitate the design and construction of advanced intelligent nanodevices.

The influence of short-time ball-milling on the stability of amorphous CoFeB alloys.

The influence of short-time milling on the atomic structure of amorphous Co(70.3)Fe(4.7)B(25) has been investigated by differential scanning calorimetry (DSC), x-ray powder diffraction (XRD), vibrating sample magnetometer (VSM) and x-ray absorption fine-structure (XAFS) techniques. Our results prove that the milling process crystallizes the initially amorphous sample and that the degree of inherent crystallization is inversely proportional to the powder particle size. The investigation of the local atomic structure documents very similar environments around the Co and Fe atoms. The high-energy ball-milling of amorphous precursor represents a practical way to prepare powders having the desired amorphous/nanocrystalline microstructure.

Structural evolution and strength change of a metallic glass at different temperatures.

The structural evolution of a Zr64.13Cu15.75Ni10.12Al10 metallic glass is investigated in-situ by high-energy synchrotron X-ray radiation upon heating up to crystallization. The structural rearrangements on the atomic scale during the heating process are analysed as a function of temperature, focusing on shift of the peaks of the structure factor in reciprocal space and the pair distribution function and radial distribution function in real space which are correlated with atomic rearrangements and progressing nanocrystallization. Thermal expansion and contraction of the coordination shells is measured and correlated with the bulk coefficient of thermal expansion. The characteristics of the microstructure and the yield strength of the metallic glass at high temperature are discussed aiming to elucidate the correlation between the atomic arrangement and the mechanical properties.

Correlation between atomic structure evolution and strength in a bulk metallic glass at cryogenic temperature.

A model Zr41.25Ti13.75Ni10Cu12.5Be22.5 (at.%) bulk metallic glass (BMG) is selected to explore the structural evolution on the atomic scale with decreasing temperature down to cryogenic level using high energy X-ray synchrotron radiation. We discover a close correlation between the atomic structure evolution and the strength of the BMG and find out that the activation energy increment of the concordantly atomic shifting at lower temperature is the main factor influencing the strength. Our results might provide a fundamental understanding of the atomic-scale structure evolution and may bridge the gap between the atomic-scale physics and the macro-scale fracture strength for BMGs.

Short range order and stability of amorphous Ge(x)Te(100-x) alloys (12 ≤ x ≤ 44.6).

Amorphous Ge(x)Te(100-x) alloys were obtained over a broad composition range (12 ≤ x ≤ 44.6) by thermal co-evaporation. Their structure was investigated by x-ray diffraction and extended x-ray absorption fine structure measurements. Experimental datasets were fitted simultaneously by the reverse Monte Carlo simulation technique. It is concluded that Te is mostly twofold coordinated and the majority of Ge atoms have four neighbours. The number of Ge-Ge and Te-Te bonds evolves monotonically with composition. Ge-Ge bonding can be observed already at x = 24 while Te-Te bonds can be found even in Ge44.6Te55.4. The models obtained by simulation show that the structure of compositions with x > 24 should be considered as a random covalent network but there is chemical ordering for x ≤ 24, exactly in the composition range where glasses can be obtained from the melt by fast quenching. The composition dependences of some physical properties also point to the connection between chemical short range order and the stability of the amorphous phase: while the glass transition temperature and microhardness increase monotonically with the composition, the thermal stability of the amorphous films goes through a maximum around x = 20-24.

Pressure dependence of magnetic properties in Fe-Mn-B amorphous alloys: evidence for inhomogeneous ferromagnetism.

The pressure dependence of the saturation magnetization and Curie temperature was studied in melt-spun Fe60Mn20B20, Fe56Mn24B20 and Fe75B25 amorphous alloys up to 0.9 GPa, corresponding to volume changes up to 0.45%. In addition, in situ high-pressure (up to 40 GPa) x-ray diffraction was performed to determine the compressibility of the latter two alloys. Both the Curie temperature TC (at atmospheric pressure TC = 201 ± 3 and 159 ± 3 K) and the low-temperature saturation magnetization M5 K,5 T decrease remarkably with increasing pressure: dTC/dp =- 31 ± 0.5 and -32 ± 5 K GPa(-1) and dlnM5 K,5 T/dp =- 0.15 ± 0.02 and -0.13 ± 0.03 GPa(-1) for xMn = 20 and 24 at.%, respectively. Compared to dlnM5 K,5 T/dp =- 0.016 ± 0.003 GPa(-1) measured for Fe75B25, the pressure dependence of M5 K,5 T is one order of magnitude larger in the ternary alloys. The bulk moduli for the Fe56Mn24B20 and Fe75B25 glasses were measured to be 152 GPa and 173 GPa, respectively. These data are also compared with the pressure dependence of the hyperfine field and theoretical calculations of the saturation moment for Fe-B alloys reported in the literature. The results were interpreted within an inhomogeneous itinerant-electron model of ferromagnetism.

Phase separation in ternary Co-Gd-Ti liquids.

The phase equilibria and the solidification behavior of ternary Co-Gd-Ti (Co ≤35 at.%) alloys have been investigated. The phase transformation and equilibria in the liquid phase were studied in situ for two alloys, Co30Gd35Ti35 and Co30Gd50Ti20, by combining electrostatic levitation of the samples with high-energy synchrotron x-ray diffraction (XRD) at elevated temperature. The XRD patterns with two diffuse maxima for molten Co30Gd35Ti35 give direct evidence for liquid-liquid phase separation in this composition. In contrast, no indication for phase separation in the Co30Gd50Ti20 alloy is detected. Coarsened microstructures, typical for the phase-separating systems, are observed for the Co30Gd35Ti35, Co25Gd37.5Ti37.5, Co10Gd45Ti45 and Co30Gd20Ti50 cast alloys. Our findings suggest that the stable miscibility gap of binary Gd-Ti extends into the ternary Co-Gd-Ti system (up to about 30 at.% Co). Thermodynamic calculations of the ternary Co-Gd-Ti system by the CALPHAD method are in good agreement with the experimental results.

Quantum mechanically guided design of Co43Fe20Ta(5.5)X(31.5) (X=B, Si, P, S) metallic glasses.

A systematic ab initio molecular dynamics study was carried out to identify valence electron concentration and size induced changes on structure, elastic and magnetic properties for Co(43)Fe(20)Ta(5.5)X(31.5) (X=B, Si, P, S). Short range order, charge transfer and the bonding nature are analyzed by means of density of states, Bader decomposition and pair distribution function analysis. A clear trend of a decrease in density and bulk modulus as well as a weaker cohesion was observed as the valence electron concentration is increased by replacing B with Si and further with P and S. These changes may be understood based on increased interatomic distances, variations in coordination numbers and the electronic structure changes; as the valence electron concentration of X is increased the X bonding becomes more ionic, which disrupts the overall metallic interactions, leading to lower cohesion and stiffness. The highest magnetic moments for the transition metals are identified for X=S, despite the fact that the presence of X generally reduces the magnetic moment of Co. Furthermore, this study reveals an extended diagonal relationship between B and P within these amorphous alloys. Based on quantum mechanical data we identify composition induced changes in short range order, charge transfer and bonding nature and link them to density, elasticity and magnetism. The interplay between transition metal d band filling and s-d hybridization was identified to be a key materials design criterion.

Ab initio molecular dynamics model for density, elastic properties and short range order of Co-Fe-Ta-B metallic glass thin films.

Density, elastic modulus and the pair distribution function of Co-Fe-Ta-B metallic glasses were obtained by ab initio molecular dynamics simulations and measured for sputtered thin films using x-ray reflectivity, nanoindentation and x-ray diffraction using high energy photons. The computationally obtained density of 8.19 g cm(-3) for Co(43)Fe(20)Ta(5.5)B(31.5) and 8.42 g cm(-3) for Co(45.5)Fe(24)Ta(6)B(24.5), as well as the Young's moduli of 273 and 251 GPa, respectively, are consistent with our experiments and literature data. These data, together with the good agreement between the theoretical and the experimental pair distribution functions, indicate that the model established here is useful to describe the density, elasticity and short range order of Co-Fe-Ta-B metallic glass thin films. Irrespective of the investigated variation in chemical composition, (Co, Fe)-B cluster formation and Co-Fe interactions are identified by density-of-states analysis. Strong bonds within the structural units and between the metallic species may give rise to the comparatively large stiffness.

Modelling the atomic structure of Al92U8 metallic glass.

The local atomic structure of the glassy Al(92)U(8) alloy was modelled by the reverse Monte Carlo (RMC) method, fitting x-ray diffraction (XRD) and extended x-ray absorption fine structure (EXAFS) signals. The final structural model was analysed by means of partial pair correlation functions, coordination number distributions and Voronoi tessellation. In our study we found that the most probable atomic separations between Al-Al and U-Al pairs in the glassy Al(92)U(8) alloy are 2.7 Å and 3.1 Å with coordination numbers 11.7 and 17.1, respectively. The Voronoi analysis did not support evidence of the existence of well-defined building blocks directly embedded in the amorphous matrix. The dense-random-packing model seems to be adequate for describing the connection between solvent and solute atoms.