Three-dimensional Imaging of Microstructure in Gold Nanocrystals

X-ray diffraction using a coherent beam involves the mutual interference among all the extremities of small crystals. The continuous diffraction pattern so produced can be phased because it can be oversampled. We have thus obtained three-dimensional images of the interiors of Au nanocrystals that show 50 nm wide bands of contrast with f111g orientation that probably arise from internal twinning by dynamic recrystallization during their formation at high temperature

Enhancement of Coherent X ray Diffraction from Nanocrystals by Introduction of X ray Optics

Coherent X-ray Diffraction is applied to investigate the structure of individual nanocrystalline silver particles in the 100nm size range. In order to enhance the available signal, Kirkpatrick-Baez focusing optics have been introduced in the 34-ID-C beamline at APS. Concerns about the preservation of coherence under these circumstances are addressed through experiment and by calculations

Reconstruction of the Shapes of Gold Nanocrystals using Coherent X-ray Diffraction

Inverse problems arise frequently in physics: The magnitude of the Fourier transform of some function is measurable, but not its phase. The “phase problem” in crystallography arises because the number of discrete measurements (Bragg peak intensities) is only half the number of unknowns (electron density points in space). Sayre first proposed that oversampling of diffraction data should allow a solution, and this has recently been demonstrated. Here we report the successful phasing of an oversampled hard x-ray diffraction pattern measured from a single nanocrystal of gold

Gaussian-Schell analysis of the transverse spatial properties of high-harmonic beams

High harmonic generation (HHG) is a compact source of coherent, ultrafast soft x-ray radiation. HHG is increasingly being used as a source to image biological and physical systems. However, many imaging techniques such as coherent diffractive imaging, and ptychography require coherent illumination. Characterization the spatial coherence of HHG sources is vital if these sources are to kind widespread applications. Here a new method for characterizing coherent radiation is used to investigate the near- and far- field spatial properties of high harmonic radiation generated in a gas cell. The intensity distribution, wavefront curvature, and complex coherence factor are measured for a range of harmonic orders, and the Gaussian-Schell model is used to determine the properties of the harmonic beam in the plane of generation. Our results show the measured spatial properties of the harmonic beam are consistent with the finite spatial coherence of the driving laser beam as well as variations of the atomic dipole phase. These findings are used to suggest new approaches for controlling and optimizing the spatial properties of light for imaging applications

Three-dimensional imaging of microstructure in Au nanocrystals.

C1 - Journal Articles RefereedX-ray diffraction using a coherent beam involves the mutual interference among all the extremities of small crystals. The continuous diffraction pattern so produced can be phased because it can be oversampled. We have thus obtained three-dimensional images of the interiors of Au nanocrystals that show 50 nm wide bands of contrast with [111] orientation that probably arise from internal twinning by dynamic recrystallization during their formation at high temperature

Synchrotron X-ray scattering and photon correlation spectroscopy studies on thin film morphology details and structural changes of an amorphous-crystalline brush diblock copolymer

We investigated structural details and temperature-induced structural changes of an amorphous-crystalline brush diblock copolymer, poly(3-((6-((7-(9H-carbazol-9-yl)heptanoyl)oxy)hexyl)thio)propylglycidyl ether)(60)-b-poly(glycidyl 12-((3,3,4,4,5,5,6,6,7,7,8,8,9,9,10,10,10-heptadecafluorodecyl)oxy)-12oxododecanoate)(20) (PGK(60)-PGF(20)) in nanoscale thin films using synchrotron grazing incidence X-ray scattering (GIXS) and X-ray photon correlation spectroscopy (XPCS). Interestingly, the diblock copolymer was found to form a mixture of two different hexagonal cylinder structures (HEX1 and HEX2) where the PGF cylinders were aligned in the film plane. HEX1 was composed of PGF cylinders with higher population of crystals while HEX2 consisted of PGF cylinders with lower population of crystals. Surprisingly, the PGF block chains favorably self-assembled because of strong lateral interactions in the bristles, forming vertical multibilayer structure with partial interdigitation even in the highly confined cylindrical geometry. In heating run up to 340 K, some fraction of HEX2 was transformed to HEX1 via cold crystallization. In contrast, HEX1 was transformed to HEX2 above 340 K because of melting of the PGF crystals. The XPCS analysis found that the HEX structural changes associated with the cold crystallization in the PGF cylinder domains took place with relatively fast dynamics. The HEX structural changes associated with melting of the PGF crystals in the cylinder domains occurred with relatively slow dynamics; this unusual dynamics of structural changes might be attributed to a high energy melting process of PGF crystals against strong lateral interactions of the bristles. (C) 2016 Elsevier Ltd. All rights reserved.1132sciescopu

Three-dimensional mapping of a deformation field inside a nanocrystal

Coherent X-ray diffraction imaging is a rapidly advancing form of microscopy: diffraction patterns, measured using the latest third-generation synchrotron radiation sources, can be inverted to obtain full three-dimensional images of the interior density within nanocrystals. Diffraction from an ideal crystal lattice results in an identical copy of this continuous diffraction pattern at every Bragg peak. This symmetry is broken by the presence of strain fields, which arise from the epitaxial contact forces that are inevitable whenever nanocrystals are prepared on a substrate. When strain is present, the diffraction copies at different Bragg peaks are no longer identical and contain additional information, appearing as broken local inversion symmetry about each Bragg point. Here we show that one such pattern can nevertheless be inverted to obtain a 'complex' crystal density, whose phase encodes a projection of the lattice deformation. A lead nanocrystal was crystallized in ultrahigh vacuum from a droplet on a silica substrate and equilibrated close to its melting point. A three-dimensional image of the density, obtained by inversion of the coherent X-ray diffraction, shows the expected facetted morphology, but in addition reveals a real-space phase that is consistent with the three-dimensional evolution of a deformation field arising from interfacial contact forces. Quantitative three-dimensional imaging of lattice strain on the nanometre scale will have profound consequences for our fundamental understanding of grain interactions and defects in crystalline materials. Our method of measuring and inverting diffraction patterns from nanocrystals represents a vital step towards the ultimate goal of atomic resolution single-molecule imaging that is a prominent justification for development of X-ray free-electron lasers