Maskless Fourier transform holography.

Fourier transform holography is a lensless imaging technique that retrieves an object's exit-wave function with high fidelity. It has been used to study nanoscale phenomena and spatio-temporal dynamics in solids, with sensitivity to the phase component of electronic and magnetic textures. However, the method requires an invasive and labor-intensive nanopatterning of a holography mask directly onto the sample, which can alter the sample properties, forces a fixed field-of-view, and leads to a low signal-to-noise ratio at high resolution. In this work, we propose using wavefront-shaping diffractive optics to create a structured probe with full control of its phase at the sample plane, circumventing the need for a mask. We demonstrate in silico that the method can image nanostructures and magnetic textures and validate our approach with a visible light-based experiment. The method enables investigation of a plethora of phenomena at the nanoscale including magnetic and electronic phase coexistence in solids, with further uses in soft and biological matter research.

Bayesian Machine Learning for Efficient Minimization of Defects in ALD Passivation Layers.

Atomic layer deposition (ALD) is an enabling technology for encapsulating sensitive materials owing to its high-quality, conformal coating capability. Finding the optimum deposition parameters is vital to achieving defect-free layers; however, the high dimensionality of the parameter space makes a systematic study on the improvement of the protective properties of ALD films challenging. Machine-learning (ML) methods are gaining credibility in materials science applications by efficiently addressing these challenges and outperforming conventional techniques. Accordingly, this study reports the ML-based minimization of defects in an ALD-Al2O3 passivation layer for the corrosion protection of metallic copper using Bayesian optimization (BO). In all experiments, BO consistently minimizes the layer defect density by finding the optimum deposition parameters in less than three trials. Electrochemical tests show that the optimized layers have virtually zero film porosity and achieve five orders of magnitude reduction in corrosion current as compared to control samples. Optimized parameters of surface pretreatment using Ar/H2 plasma, the deposition temperature above 200 °C, and 60 ms pulse time quadruple the corrosion resistance. The significant optimization of ALD layers presented in this study demonstrates the effectiveness of BO and its potential outreach to a broader audience, focusing on different materials and processes in materials science applications.

Single-frame far-field diffractive imaging with randomized illumination.

We introduce a single-frame diffractive imaging method called randomized probe imaging (RPI). In RPI, a sample is illuminated by a structured probe field containing speckles smaller than the sample's typical feature size. Quantitative amplitude and phase images are then reconstructed from the resulting far-field diffraction pattern. The experimental geometry of RPI is straightforward to implement, requires no near-field optics, and is applicable to extended samples. When the resulting data are analyzed with a complimentary algorithm, reliable reconstructions which are robust to missing data are achieved. To realize these benefits, a resolution limit associated with the numerical aperture of the probe-forming optics is imposed. RPI therefore offers an attractive modality for quantitative X-ray phase imaging when temporal resolution and reliability are critical but spatial resolution in the tens of nanometers is sufficient. We discuss the method, introduce a reconstruction algorithm, and present two proof-of-concept experiments: one using visible light, and one using soft X-rays.

Building Blocks for Magnon Optics: Emission and Conversion of Short Spin Waves.

Magnons have proven to be a promising candidate for low-power wave-based computing. The ability to encode information not only in amplitude but also in phase allows for increased data transmission rates. However, efficiently exciting nanoscale spin waves for a functional device requires sophisticated lithography techniques and therefore, remains a challenge. Here, we report on a method to measure the full spin wave isofrequency contour for a given frequency and field. A single antidot within a continuous thin film excites wave vectors along all directions within a single excitation geometry. Varying structural parameters or introducing Dzyaloshinskii-Moriya interaction allows the manipulation and control of the isofrequency contour, which is desirable for the fabrication of future magnonic devices. Additionally, the same antidot structure is utilized as a multipurpose spin wave device. Depending on its position with respect to the microstrip antenna, it can either be an emitter for short spin waves or a directional converter for incoming plane waves. Using simulations we show that such a converter structure is capable of generating a coherent spin wave beam. By introducing a short wavelength spin wave beam into existing magnonic gate logic, it is conceivable to reduce the size of devices to the micrometer scale. This method gives access to short wavelength spin waves to a broad range of magnonic devices without the need for refined sample preparation techniques. The presented toolbox for spin wave manipulation, emission, and conversion is a crucial step for spin wave optics and gate logic.

In Situ X-ray Diffraction and Spectro-Microscopic Study of ALD Protected Copper Films.

In many applications of copper in industry and research, copper migration and degradation of metallic copper to its oxides is a common problem. There are numerous ways to overcome this degradation with varying success. Atomic layer deposition (ALD) based encapsulation and passivation of the metallic copper recently emerged as a serious route to success owing to the conformality and density of the ALD films. So far, the majority of the studies have been focused on corrosion protection of copper in a variety of chemical environments, mostly at ambient temperature. An investigation of the stability of the ALD film stacks and copper's interaction with them at elevated temperatures has been lacking. Here, we study the mitigation of copper oxidation and migration in 50 nm thick Al2O3/TiO2 and Al2O3/SiO2 bilayer ALD stacks. First, the corrosion dynamics were investigated via in situ X-ray diffraction (XRD) at 350 °C under atmospheric conditions, and second, the interaction of copper with the passivation layers have been examined post factum using detailed spectro-microscopic investigations. According to the XRD results, both ALD films exhibited excellent oxidation protection. In contrast, bare Cu immediately started to oxidize at 350 °C and transformed entirely to its known oxide phases in 4 h. Spectro-microscopic studies revealed that there are structural and chemical changes on the top surface and within the film stacks. The TiO2 layer was crystallized during annealing, while the SiO2 layer stayed in the amorphous phase, which was analyzed by grazing incidence XRD and transmission electron microscopy. According to scanning electron microscopy and X-ray photoelectron spectroscopy analysis, copper was detected on the surface with a higher amount in Al2O3/TiO2 than Al2O3/SiO2, 5.2 at.% and 0.7 at.%, respectively. Based on the surface and cross-sectional analysis, copper migration was observed on both layers, albeit more substantially in Al2O3/TiO2. In the case of Al2O3/SiO2, the bulk of the copper was captured at the interface of the two oxides.

Generation and characterization of focused helical x-ray beams.

The phenomenon of orbital angular momentum (OAM) affects a variety of important applications in visible optics, including optical tweezers, free-space communication, and 3D localization for fluorescence imaging. The lack of suitable wavefront shaping optics such as spatial light modulators has inhibited the ability to impart OAM on x-ray and electron radiation in a controlled way. Here, we report the experimental observation of helical soft x-ray beams generated by holographically designed diffractive optical elements. We demonstrate that these beams rotate as a function of propagation distance and measure their vorticity and coherent mode structure using ptychography. Our results establish an approach for controlling and shaping of complex focused beams for short wavelength scanning microscopy and OAM-driven applications.

3D Nanofabrication of High-Resolution Multilayer Fresnel Zone Plates.

Focusing X-rays to single nanometer dimensions is impeded by the lack of high-quality, high-resolution optics. Challenges in fabricating high aspect ratio 3D nanostructures limit the quality and the resolution. Multilayer zone plates target this challenge by offering virtually unlimited and freely selectable aspect ratios. Here, a full-ceramic zone plate is fabricated via atomic layer deposition of multilayers over optical quality glass fibers and subsequent focused ion beam slicing. The quality of the multilayers is confirmed up to an aspect ratio of 500 with zones as thin as 25 nm. Focusing performance of the fabricated zone plate is tested toward the high-energy limit of a soft X-ray scanning transmission microscope, achieving a 15 nm half-pitch cut-off resolution. Sources of adverse influences are identified, and effective routes for improving the zone plate performance are elaborated, paving a clear path toward using multilayer zone plates in high-energy X-ray microscopy. Finally, a new fabrication concept is introduced for making zone plates with precisely tilted zones, targeting even higher resolutions.

High-throughput synthesis of modified Fresnel zone plate arrays via ion beam lithography.

Fresnel zone plates (FZP) are diffractive photonic devices used for high-resolution imaging and lithography at short wavelengths. Their fabrication requires nano-machining capabilities with exceptional precision and strict tolerances such as those enabled by modern lithography methods. In particular, ion beam lithography (IBL) is a noteworthy method thanks to its robust direct writing/milling capability. IBL allows for rapid prototyping of high-resolution FZPs that can be used for high-resolution imaging at soft X-ray energies. Here, we discuss improvements in the process enabling us to write zones down to 15 nm in width, achieving an effective outermost zone width of 30 nm. With a 35% reduction in process time and an increase in resolution by 26% compared to our previous results, we were able to resolve 21 nm features of a test sample using the FZP. The new process conditions are then applied for fabrication of large arrays of high-resolution zone plates. Results show that relatively large areas can be decorated with nanostructured devices via IBL by using multipurpose SEM/FIB instruments with potential applications in FEL focusing, extreme UV and soft X-ray lithography and as wavefront sensing devices for beam diagnostics.

3D Nanoprinted Plastic Kinoform X-Ray Optics.

High-performance focusing of X-rays requires the realization of very challenging 3D geometries with nanoscale features, sub-millimeter-scale apertures, and high aspect ratios. A particularly difficult structure is the profile of an ideal zone plate called a kinoform, which is manufactured in nonideal approximated patterns, nonetheless requires complicated multistep fabrication processes. Here, 3D fabrication of high-performance kinoforms with unprecedented aspect ratios out of low-loss plastics using femtosecond two-photon 3D nanoprinting is presented. A thorough characterization of the 3D-printed kinoforms using direct soft X-ray imaging and ptychography demonstrates superior performance with an efficiency reaching up to 20%. An extended concept is proposed for on-chip integration of various X-ray optics toward high-fidelity control of X-ray wavefronts and ultimate efficiencies even for harder X-rays. Initial results establish new, advanced focusing optics for both synchrotron and laboratory sources for a large variety of X-ray techniques and applications ranging from materials science to medicine.

Direct patterning of vortex generators on a fiber tip using a focused ion beam.

The realization of spiral phase optical elements on the cleaved end of an optical fiber by focused ion beam milling is presented. A focused Ga+ ion beam with an acceleration voltage of 30 keV is used to etch continuous spiral phase plates and fork gratings directly on the tip of the fiber. The phase characteristics of the output beam generated by the fabricated structures measured via an interference experiment confirmed the presence of phase singularity in the output beam. The devices are expected to be promising candidates for all-fiber beam shaping and optical trapping applications.

Multilayer Fresnel zone plates for high energy radiation resolve 21 nm features at 1.2 keV.

X-ray microscopy is a successful technique with applications in several key fields. Fresnel zone plates (FZPs) have been the optical elements driving its success, especially in the soft X-ray range. However, focusing of hard X-rays via FZPs remains a challenge. It is demonstrated here, that two multilayer type FZPs, delivered from the same multilayer deposit, focus both hard and soft X-rays with high fidelity. The results prove that these lenses can achieve at least 21 nm half-pitch resolution at 1.2 keV demonstrated by direct imaging, and sub-30 nm FWHM (full-pitch) resolution at 7.9 keV, deduced from autocorrelation analysis. Reported FZPs had more than 10% diffraction efficiency near 1.5 keV.

Rapid prototyping of Fresnel zone plates via direct Ga(+) ion beam lithography for high-resolution X-ray imaging.

A significant challenge to the wide utilization of X-ray microscopy lies in the difficulty in fabricating adequate high-resolution optics. To date, electron beam lithography has been the dominant technique for the fabrication of diffractive focusing optics called Fresnel zone plates (FZP), even though this preparation method is usually very complicated and is composed of many fabrication steps. In this work, we demonstrate an alternative method that allows the direct, simple, and fast fabrication of FZPs using focused Ga(+) beam lithography practically, in a single step. This method enabled us to prepare a high-resolution FZP in less than 13 min. The performance of the FZP was evaluated in a scanning transmission soft X-ray microscope where nanostructures as small as sub-29 nm in width were clearly resolved, with an ultimate cutoff resolution of 24.25 nm, demonstrating the highest first-order resolution for any FZP fabricated by the ion beam lithography technique. This rapid and simple fabrication scheme illustrates the capabilities and the potential of direct ion beam lithography (IBL) and is expected to increase the accessibility of high-resolution optics to a wider community of researchers working on soft X-ray and extreme ultraviolet microscopy using synchrotron radiation and advanced laboratory sources.

Ion beam lithography for Fresnel zone plates in X-ray microscopy.

Fresnel Zone Plates (FZP) are to date very successful focusing optics for X-rays. Established methods of fabrication are rather complex and based on electron beam lithography (EBL). Here, we show that ion beam lithography (IBL) may advantageously simplify their preparation. A FZP operable from the extreme UV to the limit of the hard X-ray was prepared and tested from 450 eV to 1500 eV. The trapezoidal profile of the FZP favorably activates its 2nd order focus. The FZP with an outermost zone width of 100 nm allows the visualization of features down to 61, 31 and 21 nm in the 1st, 2nd and 3rd order focus respectively. Measured efficiencies in the 1st and 2nd order of diffraction reach the theoretical predictions.

Efficient focusing of 8 keV X-rays with multilayer Fresnel zone plates fabricated by atomic layer deposition and focused ion beam milling.

Fresnel zone plates (FZPs) recently showed significant improvement by focusing soft X-rays down to ~10 nm. In contrast to soft X-rays, generally a very high aspect ratio FZP is needed for efficient focusing of hard X-rays. Therefore, FZPs had limited success in the hard X-ray range owing to difficulties of manufacturing high-aspect-ratio zone plates using conventional techniques. Here, employing a method of fabrication based on atomic layer deposition (ALD) and focused ion beam (FIB) milling, FZPs with very high aspect ratios were prepared. Such multilayer FZPs with outermost zone widths of 10 and 35 nm and aspect ratios of up to 243 were tested for their focusing properties at 8 keV and shown to focus hard X-rays efficiently. This success was enabled by the outstanding layer quality thanks to ALD. Via the use of FIB for slicing the multilayer structures, desired aspect ratios could be obtained by precisely controlling the thickness. Experimental diffraction efficiencies of multilayer FZPs fabricated via this combination reached up to 15.58% at 8 keV. In addition, scanning transmission X-ray microscopy experiments at 1.5 keV were carried out using one of the multilayer FZPs and resolved a 60 nm feature size. Finally, the prospective of different material combinations with various outermost zone widths at 8 and 17 keV is discussed in the light of the coupled wave theory and the thin-grating approximation. Al2O3/Ir is outlined as a promising future material candidate for extremely high resolution with a theoretical efficiency of more than 20% for as small an outermost zone width as 10 nm at 17 keV.

Sintering, microstructure, mechanical, and antimicrobial properties of HAp-ZnO biocomposites.

The implant associated infection is widely considered as a major concern in the field of biomedical applications and this has been the driving force for developing HAp-based biomaterials with antibacterial additives for possible use in prosthetic devices. In our present work, we sintered Hydroxyapatite (HAp) with different concentrations of zinc oxide microrods (ZnO) at 1250°C to produce HAp-ZnO biocomposites. In vitro antimicrobial studies were carried out to understand how ZnO addition (up to 30 wt %) to HAp leads to the improvement in bacteria static/bactericidal property and thereby, can reduce bacterial infection on implant surface. Both Gram positive (S. aureus, S. epidermidis) and Gram negative bacteria (E. coli) were used for this study. After 4 h of incubation, it was observed that microbial activity on HAp-20 wt % and HAp-30 wt % ZnO are significantly reduced in comparison to control sample, independent of type of bacterial cells. Despite such improvement in antimicrobial property, an increase in ZnO addition was found to have modest influence on fracture toughness or hardness properties. A maximum up to 1.7 MPam(1/2) indentation fracture toughness and hardness of up to 6.8 GPa were measured in HAp-ZnO biocomposites.

Hybrid processing and anisotropic sintering shrinkage in textured ZnO ceramics.

We have studied the combined effects of the templated grain growth and magnetic alignment processes on sintering, anisotropic sintering shrinkage, microstructure development and texture in ZnO ceramics. Suspensions of 0-10 vol % ZnO template particles were slip cast in a 12 T rotating magnetic field. Sintering and texture characteristics were investigated via thermomechanical analysis and electron backscatter diffraction, respectively. Sintering as well as texture characteristics depend on template concentration. For the studied ZnO system, there is a critical template concentration (2 vol % in this study) above which densification is limited by the templates owing to constrained sintering. Below this limit, the densification is enhanced and the anisotropic shrinkage is reduced, which is attributed to densifying characteristics of the templates.