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In Bragg coherent diffractive imaging, the precise location of the measured crystals in the interior of the sample is usually missing. Obtaining this information would help the study of the spatially dependent behavior of particles in the bulk of inhomogeneous samples, such as extra-thick battery cathodes. This work presents an approach to determine the 3D position of particles by precisely aligning them at the instrument axis of rotation. In the test experiment reported here, with a 60 μm-thick LiNi0.5Mn1.5O4 battery cathode, the particles were located with a precision of 20 μm in the out-of-plane direction, and the in-plane coordinates were determined with a precision of 1 μm. [ABSTRACT FROM AUTHOR]

We synthesized Ni nanoparticles with an atmospheric-thermal chemical vapor deposition method and investigated their lattice distortions and defects using Bragg coherent diffractive imaging. Because the strain can alter the magnetic properties of ferromagnetic materials, it is important to study the lattice distortion and structural imperfection. As a result of the Bragg coherent diffractive imaging, we found that the Ni nanocubes have a deformation-free zone in the middle. In addition, the defects such as dislocation and twin domain defects were detected in other Ni nanoparticles based on the Bragg diffraction images and patterns. The imaging of nanoparticles can contribute to a better understanding of their growth mechanisms and improve the design and synthesis of nanoparticles. [ABSTRACT FROM AUTHOR]

Author(s): O. G. Shpyrko (corresponding author) [1]; E. D. Isaacs [1, 3]; J. M. Logan [3]; Yejun Feng [3]; G. Aeppli [4]; R. Jaramillo [3]; H. C. Kim [3]; T. [...]

Bragg coherent diffractive imaging is a powerful technique that can be used to explore the internal structure and strain of nanoscale crystalline objects. During the data collection process, the Bragg peak typically stays within a small range of pixels on the x-ray sensitive area detector. Here, we report abrupt and irreversible Bragg peak movement during the coherent x-ray data collection process for both Pd nanocubes and a Ni nanowire. We report that this phenomenon can be attributed to x-ray momentum transfer, also known as radiation pressure, to the nanocrystals. Understanding this effect is crucial given the anticipated coherent flux increases at next-generation synchrotron sources. [ABSTRACT FROM AUTHOR]

The next generation of X-ray sources will feature highly brilliant X-ray beams that will enable the imaging of local nanoscale structures with unprecedented resolution. A general formalism to predict the achievable spatial resolution in coherent diffractive imaging, based solely on diffracted intensities, is provided. The coherent dose necessary to reach atomic resolution depends significantly on the atomic scale structure, where disordered or amorphous materials require roughly three orders of magnitude lower dose compared with the expected scaling of uniform density materials. Additionally, dose reduction for crystalline materials are predicted at certain resolutions based only on their unit-cell dimensions and structure factors. [ABSTRACT FROM AUTHOR]

We use coherent x-ray diffractive imaging to map the local distribution of strain in gold (Au) polyhedral nanocrystals grown on a silicon (Si) substrate by a single-step thermal chemical vapor deposition process. The lattice strain at the surface of the octahedral nanocrystal agrees well with the predictions of the Young-Laplace equation quantitatively, but exhibits a discrepancy near the nanocrystal-substrate interface. We attribute this discrepancy to the dissimilar interfacial energies between Au/Air and Au/Si and to the difference in thermal expansion between the nanocrystal and the substrate during the cooling process. [ABSTRACT FROM AUTHOR]

Coherent x-ray diffraction imaging is used to map the local three dimensional strain inhomogeneity and electron density distribution of two individual LiNi0.5Mn1.5O4-δ cathode nanoparticles in both ex-situ and in-situ environments. Our reconstructed images revealed a maximum strain of 0.4%. We observed different variations in strain inhomogeneity due to multiple competing effects. The compressive/tensile component of the strain is connected to the local lithium content and, on the surface, interpreted in terms of a local Jahn-Teller distortion of Mn3+. Finally, the measured strain distributions are discussed in terms of their impact on competing theoretical models of the lithiation process. [ABSTRACT FROM AUTHOR]

We have engineered an antiferromagnetic domain wall by utilizing a magnetic frustration effect of a thin iron cap layer deposited on a chromium film. Through lithography and wet etching, we selectively remove areas of the Fe cap layer to form a patterned ferromagnetic mask over the Cr film. Removing the Fe locally removes magnetic frustration in user-defined regions of the Cr film. We present x-ray microdiffraction microscopy results confirming the formation of a 90° spin-density wave propagation domain wall in Cr. This domain wall nucleates at the boundary defined by our Fe mask. [ABSTRACT FROM AUTHOR]

The surface structure of the liquid phase of the Au72Ge28 eutectic alloy has been measured using resonant and nonresonant x-ray reflectivity and grazing incidence x-ray diffraction. In spite of the significant differences in the surface tension of liquid Ge and Au the Gibbs adsorption enhancement of Ge concentration at the surface is minimal. This is in striking contrast to all the other binary alloys with large differences in the respective surface tensions measured up to date. In addition there is no evidence of the anomalous strong surface layering or in-plane crystalline order that has been reported for the otherwise quite similar liquid Au82Si18 eutectic. Instead, the surface of eutectic Au72Ge28 is liquidlike and the layering can be explained by the distorted crystal model with only slight modifications to the first layer., Engineering and Applied Sciences

A continuous surface wetting transition, pinned to a solid-liquid-liquid-vapor tetra coexistence point, is studied by x-ray reflectivity in liquid Ga-Bi binary alloys. The short-range surface potential is determined from the measured temperature evolution of the wetting film. The thermal fluctuations are shown to be insufficient to induce a noticeable breakdown of mean-field behavior, expected in short-range-interacting systems due to their \(d_u\) = 3 upper critical dimensionality., Engineering and Applied Sciences

We present X-ray reflectivity measurements from the free surface of a liquid gallium–bismuth alloy (Ga–Bi) in the temperature range close to the bulk monotectic temperature \(T_{mono}\)=222\(^\circ\)C. Our measurements indicate a continuous formation of a thick wetting film at the free surface of the binary system driven by the first order transition in the bulk at the monotectic point. We show that the behavior observed is that of a complete wetting at a tetra point of solid–liquid–liquid–vapor coexistence., Engineering and Applied Sciences

Resonant x-ray reflectivity measurements from the surface of liquid Bi22In78 find only a modest surface Bi enhancement, with 35 at.% Bi in the first atomic layer. This is in contrast to the Gibbs adsorption in all liquid alloys studied to date, which show surface segregation of a complete monolayer of the low surface tension component. This suggests that surface adsorption in Bi-In is dominated by attractive interactions that increase the number of Bi-In neighbors at the surface. These are the first measurements in which resonant x-ray scattering has been used to quantify compositional changes induced at a liquid alloy surface., Engineering and Applied Sciences

Measurements of the surface x-ray scattering from several pure liquid metals (Hg, Ga, and In) and from three alloys (Ga-Bi, Bi-In, and K-Na) with different heteroatomic chemical interactions in the bulk phase are reviewed. Surface-induced layering is found for each elemental liquid metal. The surface structure of the K-Na alloy resembles that of an elemental liquid metal. Bi-In displays pair formation at the surface. Surface segregation and a wetting film are found for Ga-Bi., Engineering and Applied Sciences

X-ray reflectivity measurements of the binary liquid Ga-Bi alloy reveal a dramatically different surface structure above and below the monotectic temperature Tmono = 222°C. A Gibbs-adsorbed Bi monolayer resides at the surface in both regimes. However, a 30Å thick, Bi-rich wetting film intrudes between the Bi monolayer and the Ga-rich bulk for T>Tmono. The wetting film's internal structure, not hitherto measured, is determined with Å resolution, showing a concentration gradient not predicted by theory and a highly diffuse interface with the bulk phase., Engineering and Applied Sciences

We report an x-ray scattering study of the microscopic structure of the surface of a liquid alkali metal. The bulk liquid structure factor of the eutectic K67Na33 alloy is characteristic of an ideal mixture, and so shares the properties of an elemental liquid alkali metal. Analysis of off-specular diffuse scattering and specular x-ray reflectivity shows that the surface roughness of the K-Na alloy follows simple capillary wave behavior with a surface structure factor indicative of surface-induced layering. Comparison of the low-angle tail of the K67Na33 surface structure factor with the one measured for liquid Ga and In previously suggests that layering is less pronounced in alkali metals. Controlled exposure of the liquid to H2 and O2 gas does not affect the surface structure, indicating that oxide and hydride are not stable at the liquid surface under these experimental conditions., Engineering and Applied Sciences

We report x-ray reflectivity (XR) and small-angle off-specular diffuse-scattering (DS) measurements from the surface of liquid indium close to its melting point of 156°C. From the XR measurements we extract the surface structure factor convolved with fluctuations in the height of the liquid surface. We present a model to describe DS that takes into account the surface structure factor, thermally excited capillary waves, and the experimental resolution. The experimentally determined DS follows this model with no adjustable parameters, allowing the surface structure factor to be deconvolved from the thermally excited height fluctuations. The resulting local electron-density profile displays exponentially decaying surface-induced layering similar to that previously reported for Ga and Hg. We compare the details of the local electron-density profiles of liquid In, which is a nearly free-electron metal, and liquid Ga, which is considerably more covalent and shows directional bonding in the melt. The oscillatory density profiles have comparable amplitudes in both metals, but surface layering decays over a length scale of 3.5±0.6Å for In and 5.5±0.4Å for Ga. Upon controlled exposure to oxygen, no oxide monolayer is formed on the liquid In surface, unlike the passivating film formed on liquid gallium., Engineering and Applied Sciences

We employ three dimensional x-ray coherent diffraction imaging to map the lattice strain distribution, and to probe the elastic properties of a single crystalline Ni (001) nanowire grown vertically on an amorphous SiO2∥Si substrate. The reconstructed density maps show that with increasing wire width, the equilibrium compressive stress in the core region decreases sharply while the surface tensile strain increases, and gradually trends to a nonzero constant. We use the retrieved projection of lattice distortion to predict the Young's Modulus of the wire based on the elasticity theory. [ABSTRACT FROM AUTHOR]

We have measured the relaxation of charge-density waves in chromium from out-of-equilibrium states achieved through rapid thermal quenching. Although pinned density waves have been predicted to relax through stick-slip dynamics, in which long-lived metastable states are linked by abrupt rearrangements of the microscopic structure, these microscopic behaviors have not been observed. Using synchrotron x rays, we have measured metastability of the order parameter and microscopic pinning phenomena including an avalanche of the charge-density wave phase. Molecular dynamical simulations based on the Fukuyama-Lee-Rice model show that these behaviors may be attributed to nucleation, pinning, and propagation of phase solitons. [ABSTRACT FROM AUTHOR]

We report on the dynamics of the structural order parameter in a chromium film using synchrotron radiation in response to photoinduced ultrafast excitations. Following transient optical excitations the effective lattice temperature of the film rises close to the Néel temperature and the charge-density wave (CDW) amplitude is reduced but does not appear to ever be fully destroyed. The persistence of the CDW diffraction signal demonstrates that the CDW, if destroyed by the laser pulse, must be reestablished within the 100-ps time resolution of the synchrotron x-ray pulses. Furthermore, at all times after photoexcitation, the CDW retains its low-temperature periodicity, rather than regenerating with its high-temperature period shortly after photoexcitation. The long-term evolution shows that the CDW reverts to its ground state on a time scale of 370 ± 40 ps. We attribute the apparent persistence of the CDW to the long-lived periodic lattice displacement in chromium. This study highlights the fundamental role of the lattice distortion and its impact on the recondensation dynamics of the charge ordered state in strongly correlated materials. [ABSTRACT FROM AUTHOR]

The resistivity of vanadium dioxide (VO2) decreased by over one order of magnitude upon localized illumination with x rays at room temperature. Despite this reduction, the structure remained in the monoclinic phase and had no signature of the high-temperature tetragonal phase that is usually associated with the lower resistance. Once illumination ceased, relaxation to the insulating state took tens of hours near room temperature. However, a full recovery of the insulating state was achieved within minutes by thermal cycling. We show that this behavior is consistent with random local-potential fluctuations and random distribution of discrete recombination sites used to model residual photoconductivity. [ABSTRACT FROM AUTHOR]

The surface dynamics of thin molten polystyrene films supported by nanoscale periodic silicon line-space gratings were investigated with x-ray photon correlation spectroscopy. Surface dynamics over these nanostructures exhibit high directional anisotropy above certain length scales, as compared to surface dynamics over flat substrates. A cutoff length scale in the dynamics perpendicular to the grooves is observed. This marks a transition from standard over-damped capillary wave behavior to suppressed dynamics due to substrate interactions. [ABSTRACT FROM AUTHOR]

We investigate the electronic and structural changes at the nanoscale in vanadium dioxide (VO2) in the vicinity of its thermally driven phase transition. Both electronic and structural changes exhibit phase coexistence leading to percolation. In addition, we observe a dichotomy between the local electronic and structural transitions. Nanoscale x-ray diffraction reveals local, nonmonotonic switching of the lattice structure, a phenomenon that is not seen in the electronic insulator-to-metal transition mapped by near-field infrared microscopy. [ABSTRACT FROM AUTHOR]

Symmetry breaking and the emergence of order is one of the most fascinating phenomena in condensed matter physics. It leads to a plethora of intriguing ground states found in antiferromagnets, Mott insulators, superconductors, and density-wave systems. Exploiting states of matter far from equilibrium can provide even more striking routes to symmetry-lowered, ordered states. Here, we demonstrate for the case of elemental chromium that moderate ultrafast photoexcitation can transiently enhance the charge-density-wave (CDW) amplitude by up to 30% above its equilibrium value, while strong excitations lead to an oscillating, large-amplitude CDW state that persists above the equilibrium transition temperature. Both effects result from dynamic electron-phonon interactions, providing an efficient mechanism to selectively transform a broad excitation of the electronic order into a well-defined, long-lived coherent lattice vibration. This mechanism may be exploited to transiently enhance order parameters in other systems with coupled degrees of freedom. [ABSTRACT FROM AUTHOR]

The structural and mechanical properties of 2D crystalline surface phases that form at the surface of liquid eutectic Au82Si18 are studied using synchrotron x-ray scattering over a large temperature range. In the vicinity of the eutectic temperature the surface consists of a 2D atomic bilayer crystalline phase that transforms into a 2D monolayer crystalline phase during heating. The latter phase eventually melts into a liquidlike surface on further heating. We demonstrate that the short wavelength capillary wave fluctuations are suppressed due to the bending rigidity of 2D crystalline phases. The corresponding reduction in the Debye-Waller factor allows for measured reflectivity to be explained in terms of an electron density profile that is consistent with the 2D surface crystals.

Elemental chromium orders antiferromagnetically near room temperature, but the ordering temperature can be driven to zero by applying large pressures. We combine diamond anvil cell and synchrotron x-ray diffraction techniques to measure directly the spin and charge order in the pure metal at the approach to its quantum critical point. Both spin and charge order are suppressed exponentially with pressure, well beyond the region where disorder cuts off such a simple evolution, and they maintain a harmonic scaling relationship over decades in scattering intensity. By comparing the development of the order parameter with that of the magnetic wave vector, it is possible to ascribe the destruction of antiferromagnetism to the growth in electron kinetic energy relative to the underlying magnetic exchange interaction.

Magnetotransport measurements on small single crystals of Cr, the elemental antiferromagnet, reveal the hysteretic thermodynamics of the domain structure. The temperature dependence of the transport coefficients is directly correlated with the real-space evolution of the domain configuration as recorded by x-ray microprobe imaging, revealing the effect of antiferromagnetic domain walls on electron transport. A single antiferromagnetic domain wall interface resistance is deduced to be of order 5 x 10(-5) mu Omega cm(2) at a temperature of 100 K.