Five-analyzer Johann spectrometer for hard X-ray photon-in/photon-out spectroscopy at the Inner Shell Spectroscopy beamline at NSLS-II: design, alignment and data acquisition.

Here, a recently commissioned five-analyzer Johann spectrometer at the Inner Shell Spectroscopy beamline (8-ID) at the National Synchrotron Light Source II (NSLS-II) is presented. Designed for hard X-ray photon-in/photon-out spectroscopy, the spectrometer achieves a resolution in the 0.5-2 eV range, depending on the element and/or emission line, providing detailed insights into the local electronic and geometric structure of materials. It serves a diverse user community, including fields such as physical, chemical, biological, environmental and materials sciences. This article details the mechanical design, alignment procedures and data-acquisition scheme of the spectrometer, with a particular focus on the continuous asynchronous data-acquisition approach that significantly enhances experimental efficiency.

2D MEMS-based multilayer Laue lens nanofocusing optics for high-resolution hard x-ray microscopy.

We report on the development of 2D integrated multilayer Laue lens (MLL) nanofocusing optics used for high-resolution x-ray microscopy. A Micro-Electro-Mechanical-Systems (MEMS) - based template has been designed and fabricated to accommodate two linear MLL optics in pre-aligned configuration. The orthogonality requirement between two MLLs has been satisfied to a better than 6 millidegrees level, and the separation along the x-ray beam direction was controlled on a micrometer scale. Developed planar 2D MLL structure has demonstrated astigmatism free point focus of ∼14 nm by ∼13 nm in horizontal and vertical directions, respectively, at 13.6 keV photon energy. Approaching 10 nm resolution with integrated 2D MLL optic is a significant step forward in applications of multilayer Laue lenses for high-resolution hard x-ray microscopy and their adoption by the general x-ray microscopy community.

Metrology of a Focusing Capillary Using Optical Ptychography.

The focusing property of an ellipsoidal monocapillary has been characterized using the ptychography method with a 405 nm laser beam. The recovered wavefront gives a 12.5×10.4µm2 focus. The reconstructed phase profile of the focused beam can be used to estimate the height error of the capillary surface. The obtained height error shows a Gaussian distribution with a standard deviation of 1.3 µm. This approach can be used as a quantitative tool for evaluating the inner functional surfaces of reflective optics, complementary to conventional metrology methods.

Large Aperture and Wedged Multilayer Laue Lens for X-ray Nanofocusing.

Diffraction optics fabricated from multilayers offer an intriguing alternative to lithography-based zone plates due to their advantages of virtually limitless aspect ratio and extremely small feature size. However, other issues, intrinsic to thin-film deposition, such as film stress and deposition rate instability, for example, limit the total achievable aperture. Over the last decade, Multilayer Laue Lens (MLLs) have progressed from a mere curiosity with initial aperture sizes in the 3-10 µm range, to real beamline-deployed optics with apertures in the 40-50 µm range (X. Huang, et al., Scientific Reports 3, 3562 (2013); E. Nazaretski, et al., Rev. Sci. Instrum. 85, 033707 (2014); E. Nazaretski, et al., Journal of Synchrotron Radiation 24, 1113 (2017)). By optimizing deposition conditions and incorporating new materials, MLLs have now broken the 100 µm thickness milestone. A flat WSi2/Al-Si MLL with a deposition thickness of 102 µm, the largest MLL to date, is reviewed. New large aperture wedged MLLs (wMLL), which were first fabricated by APS in 2006 using the WSi2/Si material system, are presented which demonstrate high focusing efficiency across a broad energy range. These results confirm findings by other groups who have also independently fabricated wMLL (A. J. Morgan, et al., Scientific Reports 5, 9892 (2015); S. Bajt, et al., Nature Light: Science and Applications 7, 17162 (2017)) based on a similar material system.

Measuring Three-Dimensional Strain and Structural Defects in a Single InGaAs Nanowire Using Coherent X-ray Multiangle Bragg Projection Ptychography.

III-As nanowires are candidates for near-infrared light emitters and detectors that can be directly integrated onto silicon. However, nanoscale to microscale variations in structure, composition, and strain within a given nanowire, as well as variations between nanowires, pose challenges to correlating microstructure with device performance. In this work, we utilize coherent nanofocused X-rays to characterize stacking defects and strain in a single InGaAs nanowire supported on Si. By reconstructing diffraction patterns from the 21̅1̅0 Bragg peak, we show that the lattice orientation varies along the length of the wire, while the strain field along the cross-section is largely unaffected, leaving the band structure unperturbed. Diffraction patterns from the 011̅0 Bragg peak are reproducibly reconstructed to create three-dimensional images of stacking defects and associated lattice strains, revealing sharp planar boundaries between different crystal phases of wurtzite (WZ) structure that contribute to charge carrier scattering. Phase retrieval is made possible by developing multiangle Bragg projection ptychography (maBPP) to accommodate coherent nanodiffraction patterns measured at arbitrary overlapping positions at multiple angles about a Bragg peak, eliminating the need for scan registration at different angles. The penetrating nature of X-ray radiation, together with the relaxed constraints of maBPP, will enable the in operando imaging of nanowire devices.

High-speed raster-scanning synchrotron serial microcrystallography with a high-precision piezo-scanner.

The Frontier Microfocus Macromolecular Crystallography (FMX) beamline at the National Synchrotron Light Source II with its 1 µm beam size and photon flux of 3 × 1012 photons s-1 at a photon energy of 12.66 keV has reached unprecedented dose rates for a structural biology beamline. The high dose rate presents a great advantage for serial microcrystallography in cutting measurement time from hours to minutes. To provide the instrumentation basis for such measurements at the full flux of the FMX beamline, a high-speed, high-precision goniometer based on a unique XYZ piezo positioner has been designed and constructed. The piezo-based goniometer is able to achieve sub-100 nm raster-scanning precision at over 10 grid-linepairs s-1 frequency for fly scans of a 200 µm-wide raster. The performance of the scanner in both laboratory and serial crystallography measurements up to the maximum frame rate of 750 Hz of the Eiger 16M's 4M region-of-interest mode has been verified in this work. This unprecedented experimental speed significantly reduces serial-crystallography data collection time at synchrotrons, allowing utilization of the full brightness of the emerging synchrotron radiation facilities.

Achieving diffraction-limited nanometer-scale X-ray point focus with two crossed multilayer Laue lenses: alignment challenges.

We discuss misalignment-induced aberrations in a pair of crossed multilayer Laue lenses used for achieving a nanometer-scale x-ray point focus. We thoroughly investigate the impacts of two most important contributions, the orthogonality and the separation distance between two lenses. We find that misalignment in the orthogonality results in astigmatism at 45° and other inclination angles when coupled with a separation distance error. Theoretical explanation and experimental verification are provided. We show that to achieve a diffraction-limited point focus, accurate alignment of the azimuthal angle is required to ensure orthogonality between two lenses, and the required accuracy is scaled with the ratio of the focus size to the aperture size.

Hard x-ray scanning imaging achieved with bonded multilayer Laue lenses.

We report scanning hard x-ray imaging with a monolithic focusing optic consisting of two multilayer Laue lenses (MLLs) bonded together. With optics pre-characterization and accurate control of the bonding process, we show that a common focal plane for both MLLs can be realized at 9.317 keV. Using bonded MLLs, we obtained a scanning transmission image of a star test pattern with a resolution of 50 × 50 nm2. By applying a ptychography algorithm, we obtained a probe size of 17 × 38 nm2 and an object image with a resolution of 13 × 13 nm2. The significant reduction in alignment complexity for bonded MLLs will greatly extend the application range in both scanning and full-field x-ray microscopies.

Achieving hard X-ray nanofocusing using a wedged multilayer Laue lens.

We report on the fabrication and the characterization of a wedged multilayer Laue lens for x-ray nanofocusing. The lens was fabricated using a sputtering deposition technique, in which a specially designed mask was employed to introduce a thickness gradient in the lateral direction of the multilayer. X-ray characterization shows an efficiency of 27% and a focus size of 26 nm at 14.6 keV, in a good agreement with theoretical calculations. These results indicate that the desired wedging is achieved in the fabricated structure. We anticipate that continuous development on wedged MLLs will advance x-ray nanofocusing optics to new frontiers and enrich capabilities and opportunities for hard X-ray microscopy.

A high-precision instrument for mapping of rotational errors in rotary stages.

A rotational stage is a key component of every X-ray instrument capable of providing tomographic or diffraction measurements. To perform accurate three-dimensional reconstructions, runout errors due to imperfect rotation (e.g. circle of confusion) must be quantified and corrected. A dedicated instrument capable of full characterization and circle of confusion mapping in rotary stages down to the sub-10 nm level has been developed. A high-stability design, with an array of five capacitive sensors, allows simultaneous measurements of wobble, radial and axial displacements. The developed instrument has been used for characterization of two mechanical stages which are part of an X-ray microscope.

Micromachined Silicon Platform for Precise Assembly of 2D Multilayer Laue Lenses for High-Resolution X-ray Microscopy.

We report on a developed micromachined silicon platform for the precise assembly of 2D multilayer Laue lenses (MLLs) for high-resolution X-ray microscopy. The platform is 10 × 10 mm2 and is fabricated on ~500 µm thick silicon wafers through multiple steps of photolithography and deep reactive-ion etching. The platform accommodates two linear MLLs in a pre-defined configuration with precise angular and lateral position control. In this work, we discuss the design and microfabrication of the platform, and characterization regarding MLLs assembly, position control, repeatability, and stability. The results demonstrate that a micromachined platform can be used for the assembly of a variety of MLLs with different dimensions and optical parameters. The angular misalignment of 2D MLLs is well controlled in the range of the designed accuracy, down to a few millidegrees. The separation distance between MLLs is adjustable from hundreds to more than one thousand micrometers. The use of the developed platform greatly simplifies the alignment procedure of the MLL optics and reduces the complexity of the X-ray microscope. It is a significant step forward for the development of monolithic 2D MLL nanofocusing optics for high-resolution X-ray microscopy.

Tunable hard x-ray nanofocusing with Fresnel zone plates fabricated using deep etching.

Fresnel zone plates are widely used for x-ray nanofocusing, due to their ease of alignment and energy tunability. Their spatial resolution is limited in part by their outermost zone width dr N , while their efficiency is limited in part by their thickness t zp. We demonstrate the use of Fresnel zone plate optics for x-ray nanofocusing with dr N = 16 nm outermost zone width and a thickness of about t zp = 1.8 µm (or an aspect ratio of 110) with an absolute focusing efficiency of 4.7% at 12 keV, and 6.2% at 10 keV. Using partially coherent illumination at 12 keV, the zone plate delivered a FWHM focus of 46 × 60 nm at 12 keV, with the first order coherent mode in a ptychographic reconstruction showing a probe size of 16 nm FWHM. These optics were fabricated using a combination of metal assisted chemical etching and atomic layer deposition for the diffracting structures, and silicon wafer back-thinning to produce optics useful for real applications. This approach should enable new higher resolution views of thick materials, especially when energy tunability is required.

Ptychographic X-ray speckle tracking with multi-layer Laue lens systems.

The ever-increasing brightness of synchrotron radiation sources demands improved X-ray optics to utilize their capability for imaging and probing biological cells, nano-devices and functional matter on the nanometre scale with chemical sensitivity. Hard X-rays are ideal for high-resolution imaging and spectroscopic applications owing to their short wavelength, high penetrating power and chemical sensitivity. The penetrating power that makes X-rays useful for imaging also makes focusing them technologically challenging. Recent developments in layer deposition techniques have enabled the fabrication of a series of highly focusing X-ray lenses, known as wedged multi-layer Laue lenses. Improvements to the lens design and fabrication technique demand an accurate, robust, in situ and at-wavelength characterization method. To this end, a modified form of the speckle tracking wavefront metrology method has been developed. The ptychographic X-ray speckle tracking method is capable of operating with highly divergent wavefields. A useful by-product of this method is that it also provides high-resolution and aberration-free projection images of extended specimens. Three separate experiments using this method are reported, where the ray path angles have been resolved to within 4 nrad with an imaging resolution of 45 nm (full period). This method does not require a high degree of coherence, making it suitable for laboratory-based X-ray sources. Likewise, it is robust to errors in the registered sample positions, making it suitable for X-ray free-electron laser facilities, where beam-pointing fluctuations can be problematic for wavefront metrology.

Perovskite neural trees.

Trees are used by animals, humans and machines to classify information and make decisions. Natural tree structures displayed by synapses of the brain involves potentiation and depression capable of branching and is essential for survival and learning. Demonstration of such features in synthetic matter is challenging due to the need to host a complex energy landscape capable of learning, memory and electrical interrogation. We report experimental realization of tree-like conductance states at room temperature in strongly correlated perovskite nickelates by modulating proton distribution under high speed electric pulses. This demonstration represents physical realization of ultrametric trees, a concept from number theory applied to the study of spin glasses in physics that inspired early neural network theory dating almost forty years ago. We apply the tree-like memory features in spiking neural networks to demonstrate high fidelity object recognition, and in future can open new directions for neuromorphic computing and artificial intelligence.

Resolving 500 nm axial separation by multi-slice X-ray ptychography.

Multi-slice X-ray ptychography offers an approach to achieve images with a nanometre-scale resolution from samples with thicknesses larger than the depth of field of the imaging system by modeling a thick sample as a set of thin slices and accounting for the wavefront propagation effects within the specimen. Here, we present an experimental demonstration that resolves two layers of nanostructures separated by 500 nm along the axial direction, with sub-10 nm and sub-20 nm resolutions on two layers, respectively. Fluorescence maps are simultaneously measured in the multi-modality imaging scheme to assist in decoupling the mixture of low-spatial-frequency features across different slices. The enhanced axial sectioning capability using correlative signals obtained from multi-modality measurements demonstrates the great potential of the multi-slice ptychography method for investigating specimens with extended dimensions in 3D with high resolution.

Design, characterization, and performance of a hard x-ray transmission microscope at the National Synchrotron Light Source II 18-ID beamline.

A transmission X-ray microscope has been designed and commissioned at the 18-ID Full-field X-ray Imaging beamline at the National Synchrotron Light Source II. This instrument operates in the 5-11 keV range, and, with the current set of optics, is capable of 30 nm spatial resolution imaging, with a field of view of about 40 µm. For absorption contrast, the minimum exposure time for a single projection image is about 20 ms and an entire 3D tomography data set can be acquired in under 1 min. The system enables tomographic reconstructions with sub-50 nm spatial resolution without the use of markers on the sample or corrections for rotation run-outs.

Nanospectroscopy Captures Nanoscale Compositional Zonation in Barite Solid Solutions.

Scientists have long suspected that compositionally zoned particles can form under far-from equilibrium precipitation conditions, but their inferences have been based on bulk solid and solution measurements. We are the first to directly observe nanoscale trace element compositional zonation in <10 µm-sized particles using X-ray fluorescence nanospectroscopy at the Hard X-ray Nanoprobe (HXN) Beamline at National Synchrotron Light Source II (NSLS-II). Through high-resolution images, compositional zonation was observed in barite (BaSO4) particles precipitated from aqueous solution, in which Sr2+ cations as well as HAsO42- anions were co-precipitated into (Ba,Sr)SO4 or Ba(SO4,HAsO4) solid solutions. Under high salinity conditions (NaCl ≥ 1.0 M), bands contained ~3.5 to ~5 times more trace element compared to the center of the particle formed in early stages of particle growth. Quantitative analysis of Sr and As fractional substitution allowed us to determine that different crystallographic growth directions incorporated trace elements to different extents. These findings provide supporting evidence that barite solid solutions have great potential for trace element incorporation; this has significant implications for environmental and engineered systems that remove hazardous substances from water.

X-ray focusing with efficient high-NA multilayer Laue lenses.

Multilayer Laue lenses are volume diffraction elements for the efficient focusing of X-rays. With a new manufacturing technique that we introduced, it is possible to fabricate lenses of sufficiently high numerical aperture (NA) to achieve focal spot sizes below 10 nm. The alternating layers of the materials that form the lens must span a broad range of thicknesses on the nanometer scale to achieve the necessary range of X-ray deflection angles required to achieve a high NA. This poses a challenge to both the accuracy of the deposition process and the control of the materials properties, which often vary with layer thickness. We introduced a new pair of materials-tungsten carbide and silicon carbide-to prepare layered structures with smooth and sharp interfaces and with no material phase transitions that hampered the manufacture of previous lenses. Using a pair of multilayer Laue lenses (MLLs) fabricated from this system, we achieved a two-dimensional focus of 8.4 × 6.8 nm2 at a photon energy of 16.3 keV with high diffraction efficiency and demonstrated scanning-based imaging of samples with a resolution well below 10 nm. The high NA also allowed projection holographic imaging with strong phase contrast over a large range of magnifications. An error analysis indicates the possibility of achieving 1 nm focusing.

Multimodality hard-x-ray imaging of a chromosome with nanoscale spatial resolution.

We developed a scanning hard x-ray microscope using a new class of x-ray nano-focusing optic called a multilayer Laue lens and imaged a chromosome with nanoscale spatial resolution. The combination of the hard x-ray's superior penetration power, high sensitivity to elemental composition, high spatial-resolution and quantitative analysis creates a unique tool with capabilities that other microscopy techniques cannot provide. Using this microscope, we simultaneously obtained absorption-, phase-, and fluorescence-contrast images of Pt-stained human chromosome samples. The high spatial-resolution of the microscope and its multi-modality imaging capabilities enabled us to observe the internal ultra-structures of a thick chromosome without sectioning it.

Fly-scan ptychography.

We report an experimental ptychography measurement performed in fly-scan mode. With a visible-light laser source, we demonstrate a 5-fold reduction of data acquisition time. By including multiple mutually incoherent modes into the incident illumination, high quality images were successfully reconstructed from blurry diffraction patterns. This approach significantly increases the throughput of ptychography, especially for three-dimensional applications and the visualization of dynamic systems.