G. Brian Stephenson

Focusing of hard x-rays to 16 nanometers with a multilayer Laue lens

We report improved results for hard x-ray focusing using a multilayer Laue lens MLL. We have measured a line focus of 16 nm width with an efficiency of 31% at a wavelength =0.064 nm 19.5 keV using a partial MLL structure with an outermost zone width of 5 nm. The results are in good agreement with the theoretically predicted performance.

A hard X-ray nanoprobe beamline for nanoscale microscopy

The Hard X-ray Nanoprobe Beamline is a precision platform for scanning probe and full-field microscopy with 3–30 keV X-rays. A combination of high-stability X-ray optics and precision motion sensing and control enables detailed studies of the internal features of samples with resolutions approaching 30 nm.

Takagi-Taupin description of x-ray dynamical diffraction from diffractive optics with large numerical aperture

We present a formalism of x-ray dynamical diffraction from volume diffractive optics with large numerical aperture and high aspect ratio, in an analogy to the Takagi-Taupin equations [Acta Crystallogr. 15, 1311 (1962); Bull. Soc. Fr. Mineral. Crystallogr. 87, 469 (1964)] for strained single crystals. We derive a set of basic equations for dynamical diffraction from volume diffractive optics, which enable us to study the focusing property of these optics with various grating profiles. We study volume diffractive optics that satisfy the Bragg condition to various degrees, namely, flat, tilted, and wedged geometries, and derive the curved geometries required for ultimate focusing. We show that the curved geometries satisfy both the Bragg condition everywhere and phase requirement for point focusing and effectively focus hard x rays to a scale close to the wavelength. Our calculations were made for an x-ray wavelength of 0.064 nm (19.5 keV).

Two dimensional hard x-ray nanofocusing with crossed multilayer Laue lenses

Hard x-ray microscopy with nanometer resolution will open frontiers in the study of materials and devices, environmental sciences, and life sciences by utilizing the unique characterization capabilities of x-rays. Here we report two-dimensional nanofocusing by multilayer Laue lenses (MLLs), a type of diffractive optics that is in principle capable of focusing x-rays to 1 nm. We demonstrate focusing to a 25 × 27 nm(2) FWHM spot with an efficiency of 2% at a photon energy of 12 keV, and to a 25 × 40 nm(2) FWHM spot with an efficiency of 17% at a photon energy of 19.5 keV.

Wedged multilayer Laue lens

A multilayer Laue lens (MLL) is an x-ray focusing optic fabricated from a multilayer structure consisting of thousands of layers of two different materials produced by thin-film deposition. The sequence of layer thicknesses is controlled to satisfy the Fresnel zone plate law and the multilayer is sectioned to form the optic. An improved MLL geometry can be created by growing each layer with an in-plane thickness gradient to form a wedge, so that every interface makes the correct angle with the incident beam for symmetric Bragg diffraction. The ultimate hard x-ray focusing performance of a wedged MLL has been predicted to be significantly better than that of a nonwedged MLL, giving subnanometer resolution with high efficiency. Here, we describe a method to deposit the multilayer structure needed for an ideal wedged MLL and report our initial deposition results to produce these structures.

Sectioning of multilayers to make a multilayer Laue lens

We report a process to fabricate multilayer Laue lenses (MLLs) by sectioning and thinning multilayer films. This method can produce a linear zone plate structure with a very large ratio of zone depth to width (e.g., >1000), orders of magnitude larger than can be attained with photolithography. Consequently, MLLs are advantageous for efficient nanofocusing of hard x rays. MLL structures prepared by the technique reported here have been tested at an x-ray energy of 19.5 keV, and a diffraction-limited performance was observed. The present article reports the fabrication techniques that were used to make the MLLs.

Stoichiometry optimization of homoepitaxial oxide thin films using x-ray diffraction

Homoepitaxial SrTiO3 thin films grown by molecular beam epitaxy are analyzed using high-resolution x-ray diffraction and transmission electron microscopy. Measured 00L x-ray scans from stoichiometric and nonstoichiometric films are compared with calculations that account for the effects of film thickness, lattice parameter, fractional site occupancy, and an offset between film and substrate at the interface. It is found that thickness fringes, commonly observed around Bragg reflections even in stoichiometric homoepitaxial SrTiO3 films, arise from a film/substrate interface offset. Transmission electron microscopy studies confirm the presence of strain at those homoepitaxial interfaces that show an offset in x-ray diffraction. The consequences for stoichiometry optimization of homoepitaxial films using high-resolution x-ray diffraction and the quality of regrown oxide interfaces are discussed.

Bragg coherent diffractive imaging of single-grain defect dynamics in polycrystalline films

Watching defects in heated thin films The response of materials to external conditions depends on small-scale features such as defects and grain boundaries. Yau et al. heated gold thin films and used coherent x-ray diffractive imaging to track how these microstructures developed during grain growth (see the Perspective by Suter). The technique allowed nondestructive visualization of the features in three dimensions. The method should help link external stimuli to material response through changes in microstructure, thereby allowing development of novel materials through microstructural engineering. Science, this issue p. 739; see also p. 704 Bragg coherent diffractive imaging can track defects and grain boundaries during heating in a gold thin film. Polycrystalline material properties depend on the distribution and interactions of their crystalline grains. In particular, grain boundaries and defects are crucial in determining their response to external stimuli. A long-standing challenge is thus to observe individual grains, defects, and strain dynamics inside functional materials. Here we report a technique capable of revealing grain heterogeneity, including strain fields and individual dislocations, that can be used under operando conditions in reactive environments: grain Bragg coherent diffractive imaging (gBCDI). Using a polycrystalline gold thin film subjected to heating, we show how gBCDI resolves grain boundary and dislocation dynamics in individual grains in three-dimensional detail with 10-nanometer spatial and subangstrom displacement field resolution. These results pave the way for understanding polycrystalline material response under external stimuli and, ideally, engineering particular functions.

Oxidation of PtNi nanoparticles studied by a scanning X-ray fluorescence microscope with multi-layer Laue lenses

We report a study of the oxidation process of individual PtNi nanoparticles (NPs) conducted with a novel scanning multi-layer Laue lens X-ray microscope. The elemental maps reveal that alloyed PtNi NPs were transformed into Pt/NiO core-shell NPs by thermal oxidation. The observations furthermore indicate that a coalescence of Pt/NiO core-shell NPs occurred during oxidation.

Observation of the polarization of domains in ferroelectric thin films using x-ray interference

We report that the sign of the polarization of an epitaxial ferroelectric film can be determined from the interference between the x-ray scattering from the film and the substrate. X-ray scattering measurements of a 10 nm epitaxial PbTiO3 film grown by metal-organic chemical vapor deposition on a SrTiO3 substrate are presented. The scattering profile near the 001 peaks of the film and substrate shows clear evidence of the interference effects. Analysis indicates that this film is a single domain of specific polarity.