Compact single-shot soft X-ray photon spectrometer for free-electron laser diagnostics.

The photon spectrum from free-electron laser (FEL) light sources offers valuable information in time-resolved experiments and machine optimization in the spectral and temporal domains. We have developed a compact single-shot photon spectrometer to diagnose soft X-ray spectra. The spectrometer consists of an array of off-axis Fresnel zone plates (FZP) that act as transmission-imaging gratings, a Ce:YAG scintillator, and a microscope objective to image the scintillation target onto a two-dimensional imaging detector. This spectrometer operates in segmented energy ranges which covers tens of electronvolts for each absorption edge associated with several atomic constituents: carbon, nitrogen, oxygen, and neon. The spectrometer's performance is demonstrated at a repetition rate of 120 Hz, but our detection scheme can be easily extended to 200 kHz spectral collection by employing a fast complementary metal oxide semiconductor (CMOS) line-scan camera to detect the light from the scintillator. This compact photon spectrometer provides an opportunity for monitoring the spectrum downstream of an endstation in a limited space environment with sub-electronvolt energy resolution.

Prediction on X-ray output of free electron laser based on artificial neural networks.

Knowledge of x-ray free electron lasers' (XFELs) pulse characteristics delivered to a sample is crucial for ensuring high-quality x-rays for scientific experiments. XFELs' self-amplified spontaneous emission process causes spatial and spectral variations in x-ray pulses entering a sample, which leads to measurement uncertainties for experiments relying on multiple XFEL pulses. Accurate in-situ measurements of x-ray wavefront and energy spectrum incident upon a sample poses challenges. Here we address this by developing a virtual diagnostics framework using an artificial neural network (ANN) to predict x-ray photon beam properties from electron beam properties. We recorded XFEL electron parameters while adjusting the accelerator's configurations and measured the resulting x-ray wavefront and energy spectrum shot-to-shot. Training the ANN with this data enables effective prediction of single-shot or average x-ray beam output based on XFEL undulator and electron parameters. This demonstrates the potential of utilizing ANNs for virtual diagnostics linking XFEL electron and photon beam properties.

Novel fabrication tools for dynamic compression targets with engineered voids using photolithography methods.

Mesoscale imperfections, such as pores and voids, can strongly modify the properties and the mechanical response of materials under extreme conditions. Tracking the material response and microstructure evolution during void collapse is crucial for understanding its performance. In particular, imperfections in the ablator materials, such as voids, can limit the efficiency of the fusion reaction and ultimately hinder ignition. To characterize how voids influence the response of materials during dynamic loading and seed hydrodynamic instabilities, we have developed a tailored fabrication procedure for designer targets with voids at specific locations. Our procedure uses SU-8 as a proxy for the ablator materials and hollow silica microspheres as a proxy for voids and pores. By using photolithography to design the targets' geometry, we demonstrate precise and highly reproducible placement of a single void within the sample, which is key for a detailed understanding of its behavior under shock compression. This fabrication technique will benefit high-repetition rate experiments at x-ray and laser facilities. Insight from shock compression experiments will provide benchmarks for the next generation of microphysics modeling.

Wavefront preserving and high efficiency diamond grating beam splitter for x-ray free electron laser.

X-ray free electron lasers (XFELs) provide femtosecond high-power x-ray beams with high spatial coherence, resulting in numerous influential discoveries. Diffractive optics allow for the easy manipulation and measurement of an x-ray beam's wavefront and enable the realization of complex designed properties and specifications. For example, phase gratings can be used as x-ray beam splitters to enable beam sharing by multiple end stations or in-situ beam monitoring, including spectrum and wavefront measurements. Wavefront preservation and high efficiency and survivability under high power are requirements for such beam splitters. Diamond is the most suitable choice for phase grating fabrication, due to its high thermal conductivity that enables it to survive high average power XFEL beams. We have fabricated a large area (2×2 mm2) high aspect ratio (13:1) diamond grating on a diamond plate. Testing was performed at 9.5 keV and resulted in a high splitting efficiency (30%). Tunable efficiency was obtained via tilting the grating with respect to the x-ray beam. Wavefront fidelity of the split beams were measured to less than λ/100 using a Talbot wavefront sensor.

X-ray free-electron laser wavefront sensing using the fractional Talbot effect.

Wavefront sensing at X-ray free-electron lasers is important for quantitatively understanding the fundamental properties of the laser, for aligning X-ray instruments and for conducting scientific experimental analysis. A fractional Talbot wavefront sensor has been developed. This wavefront sensor enables measurements over a wide range of energies, as is common on X-ray instruments, with simplified mechanical requirements and is compatible with the high average power pulses expected in upcoming X-ray free-electron laser upgrades. Single-shot measurements were performed at 500 eV, 1000 eV and 1500 eV at the Linac Coherent Light Source. These measurements were applied to study both mirror alignment and the effects of undulator tapering schemes on source properties. The beamline focal plane position was tracked to an uncertainty of 0.12 mm, and the source location for various undulator tapering schemes to an uncertainty of 1 m, demonstrating excellent sensitivity. These findings pave the way to use the fractional Talbot wavefront sensor as a routine, robust and sensitive tool at X-ray free-electron lasers as well as other high-brightness X-ray sources.

Metal-Assisted Chemical Etching and Electroless Deposition for Fabrication of Hard X-ray Pd/Si Zone Plates.

Zone plates are diffractive optics commonly used in X-ray microscopes. Here, we present a wet-chemical approach for fabricating high aspect ratio Pd/Si zone plate optics aimed at the hard X-ray regime. A Si zone plate mold is fabricated via metal-assisted chemical etching (MACE) and further metalized with Pd via electroless deposition (ELD). MACE results in vertical Si zones with high aspect ratios. The observed MACE rate with our zone plate design is 700 nm/min. The ELD metallization yields a Pd density of 10.7 g/cm 3 , a value slightly lower than the theoretical density of 12 g/cm 3 . Fabricated zone plates have a grid design, 1:1 line-to-space-ratio, 30 nm outermost zone width, and an aspect ratio of 30:1. At 9 keV X-ray energy, the zone plate device shows a first order diffraction efficiency of 1.9%, measured at the MAX IV NanoMAX beamline. With this work, the possibility is opened to fabricate X-ray zone plates with low-cost etching and metallization methods.

Wavefront sensing at X-ray free-electron lasers.

Here a direct comparison is made between various X-ray wavefront sensing methods with application to optics alignment and focus characterization at X-ray free-electron lasers (XFELs). Focus optimization at XFEL beamlines presents unique challenges due to high peak powers as well as beam pointing instability, meaning that techniques capable of single-shot measurement and that probe the wavefront at an out-of-focus location are desirable. The techniques chosen for the comparison include single-phase-grating Talbot interferometry (shearing interferometry), dual-grating Talbot interferometry (moiré deflectometry) and speckle tracking. All three methods were implemented during a single beam time at the Linac Coherent Light Source, at the X-ray Pump Probe beamline, in order to make a direct comparison. Each method was used to characterize the wavefront resulting from a stack of beryllium compound refractive lenses followed by a corrective phase plate. In addition, difference wavefront measurements with and without the phase plate agreed with its design to within λ/20, which enabled a direct quantitative comparison between methods. Finally, a path toward automated alignment at XFEL beamlines using a wavefront sensor to close the loop is presented.

Shaping coherent x-rays with binary optics.

Diffractive lenses fabricated by lithographic methods are one of the most popular image forming optics in the x-ray regime. Most commonly, binary diffractive optics, such as Fresnel zone plates, are used due to their ability to focus at high resolution and to manipulate the x-ray wavefront. We report here a binary zone plate design strategy to form arbitrary illuminations for coherent multiplexing, structured illumination, and wavefront shaping experiments. Given a desired illumination, we adjust the duty cycle, harmonic order, and zone placement to vary both the amplitude and phase of the wavefront at the lens. This enables the binary lithographic pattern to generate arbitrary structured illumination optimized for a variety of applications such as holography, interferometry, ptychography, imaging, and others.

Focal Spot and Wavefront Sensing of an X-Ray Free Electron laser using Ronchi shearing interferometry.

The Linac Coherent Light Source (LCLS) is an X-ray source of unmatched brilliance, that is advancing many scientific fields at a rapid pace. The highest peak intensities that are routinely produced at LCLS take place at the Coherent X-ray Imaging (CXI) instrument, which can produce spotsize at the order of 100 nm, and such spotsizes and intensities are crucial for experiments ranging from coherent diffractive imaging, non-linear x-ray optics and high field physics, and single molecule imaging. Nevertheless, a full characterisation of this beam has up to now not been performed. In this paper we for the first time characterise this nanofocused beam in both phase and intensity using a Ronchi Shearing Interferometric technique. The method is fast, in-situ, uses a straightforward optimization algoritm, and is insensitive to spatial jitter.

Ultra-high aspect ratio high-resolution nanofabrication for hard X-ray diffractive optics.

Although diffractive optics have played a major role in nanoscale soft X-ray imaging, high-resolution and high-efficiency diffractive optics have largely been unavailable for hard X-rays where many scientific, technological and biomedical applications exist. This is owing to the long-standing challenge of fabricating ultra-high aspect ratio high-resolution dense nanostructures. Here we report significant progress in ultra-high aspect ratio nanofabrication of high-resolution, dense silicon nanostructures using vertical directionality controlled metal-assisted chemical etching. The resulting structures have very smooth sidewalls and can be used to pattern arbitrary features, not limited to linear or circular. We focus on the application of X-ray zone plate fabrication for high-efficiency, high-resolution diffractive optics, and demonstrate the process with linear, circular, and spiral zone plates. X-ray measurements demonstrate high efficiency in the critical outer layers. This method has broad applications including patterning for thermoelectric materials, battery anodes and sensors among others.

Extreme ultraviolet laser-based table-top aerial image metrology of lithographic masks.

We have realized the first demonstration of a table-top aerial imaging microscope capable of characterizing pattern and defect printability in extreme ultraviolet lithography masks. The microscope combines the output of a 13.2 nm wavelength, table-top, plasma-based, EUV laser with zone plate optics to mimic the imaging conditions of an EUV lithographic stepper. We have characterized the illumination of the system and performed line-edge roughness measurements on an EUVL mask. The results open a path for the development of a compact aerial imaging microscope for high-volume manufacturing.

Sacrificial tamper slows down sample explosion in FLASH diffraction experiments.

Intense and ultrashort x-ray pulses from free-electron lasers open up the possibility for near-atomic resolution imaging without the need for crystallization. Such experiments require high photon fluences and pulses shorter than the time to destroy the sample. We describe results with a new femtosecond pump-probe diffraction technique employing coherent 0.1 keV x rays from the FLASH soft x-ray free-electron laser. We show that the lifetime of a nanostructured sample can be extended to several picoseconds by a tamper layer to dampen and quench the sample explosion, making <1 nm resolution imaging feasible.

Phase contrast soft x-ray microscopy using Zernike zone plates.

Soft x-ray Zernike phase contrast microscopy was implemented using a "Zernike zone plate" (ZZP) without the use of a separate phase filter in the back focal plane. The ZZP is a single optic that integrates the appropriate +/-pi/2 radians phase shift through selective zone placement shifts in a Fresnel zone plate. Imaging using a regular zone plate, positive ZZP, and negative ZZP was performed at a wavelength of lambda = 2.163 nm. Contrast enhancement with the positive ZZP and contrast reversal with the negative ZZP were observed.

High numerical aperture tabletop soft x-ray diffraction microscopy with 70-nm resolution.

Light microscopy has greatly advanced our understanding of nature. The achievable resolution, however, is limited by optical wavelengths to approximately 200 nm. By using imaging and labeling technologies, resolutions beyond the diffraction limit can be achieved for specialized specimens with techniques such as near-field scanning optical microscopy, stimulated emission depletion microscopy, and photoactivated localization microscopy. Here, we report a versatile soft x-ray diffraction microscope with 70- to 90-nm resolution by using two different tabletop coherent soft x-ray sources-a soft x-ray laser and a high-harmonic source. We also use field curvature correction that allows high numerical aperture imaging and near-diffraction-limited resolution of 1.5lambda. A tabletop soft x-ray diffraction microscope should find broad applications in biology, nanoscience, and materials science because of its simple optical design, high resolution, large depth of field, 3D imaging capability, scalability to shorter wavelengths, and ultrafast temporal resolution.

Soft-X-ray microscopy using spiral zone plates.

Phase sensitive soft-x-ray microscopy methods enable the study of specimens for which phase effects are a prevalent contrast mechanism. One way to detect these phase effects is to optically implement the radial Hilbert transform by using spiral zone plates (SZPs), which results in the isotropic measurement of the amplitude and phase gradient in a sample. Soft-x-ray microscopy using an SZP as a single element objective lens was demonstrated through the imaging of a 1 microm circular aperture at a wavelength of 2.73 nm(454 eV). A regular zone plate, a charge 1 SZP, and a charge 2 SZP were fabricated using electron beam lithography and were used as the imaging optic in the microscopy setup. The charge 1 and charge 2 SZP images exhibited isotropic edge enhancement as a result of radial Hilbert filtering.

Single-element objective lens for soft x-ray differential interference contrast microscopy.

High-resolution soft x-ray differential interference contrast (DIC) imaging was demonstrated through the use of a single-element objective, the XOR pattern, in a full-field soft x-ray microscope. DIC images of the magnetic domains in a 59 nm thick amorphous Gd25Fe75 layer were obtained and magnetic phase contributions were directly imaged. With its elemental, chemical, and magnetic specificity, compatibility with various sample environments, and ease of implementation, we expect this soft x-ray DIC technique to become one of the standard modes of operation for existing full-field soft x-ray microscopes.

Dual-modality imaging of function and physiology.

Dual-modality imaging is a technique in which computed tomography (CT) or magnetic resonance imaging is combined with positron emission tomography or single-photon emission CT to acquire structural and functional images with an integated system. The data are acquired in a single procedure; the patient remains on the scanner table while undergoing both x-ray and radionuclide studies to facilitate correlation between the structural and functional images. The resulting data can aid in localization, enabling more specific diagnosis than can be obtained with a conventional imaging study. In addition, the anatomic information can be used to compensate the correlated radionuclide data for physical perturbations such as photon attenuation, scatter radiation, and partial volume errors. Thus, dual-modality imaging provides a priori information that can improve both the visual quality and the quantitative accuracy of the radionuclide images. Dual-modality imaging systems are also being developed for biologic research involving small animals. Small-animal dual-modality systems offer advantages for measurements that currently are performed invasively with autoradiography and tissue sampling. By acquiring data noninvasively, dual-modality imaging permits serial studies in a single animal, enables measurements to be performed with fewer animals, and improves the statistical quality of the data.

Dual-modality imaging of cancer with SPECT/CT.

Dual-modality imaging is an in vivo diagnostic technique that obtains structural and functional information directly from patient studies in a way that cannot be achieved with separate imaging systems alone. Dual-modality imaging systems are configured by combining computed tomography (CT) with radionuclide imaging (using positron emission tomography (PET) or single-photon emission computed tomography (SPECT)) on a single gantry which allows both functional and structural imaging to be performed during a single imaging session without having the patient leave the imaging system. A SPECT/CT system developed at UCSF is being used in a study to determine if dual-modality imaging offers advantages for assessment of patients with prostate cancer using (111)In-ProstaScint, a radiolabeled antibody for the prostate-specific membrane antigen. (111)In-ProstaScint images are reconstructed using an iterative maximum-likelihood expectation-maximization (ML-EM) algorithm with correction for photon attenuation using a patient-specific map of attenuation coefficients derived from CT. The ML-EM algorithm accounts for the dual-photon nature of the 111In-labeled radionuclide, and incorporates correction for the geometric response of the radionuclide collimator. The radionuclide image then can be coregistered and overlaid in color on a grayscale CT image for improved localization of the functional information from SPECT. Radionuclide images obtained with SPECT/CT and reconstructed using ML-EM with correction for photon attenuation and collimator response improve image quality in comparison to conventional radionuclide images obtained with filtered backprojection reconstruction. These results illustrate the potential advantages of dual-modality imaging for improving the quality and the localization of radionuclide uptake for staging disease, planning treatment, and monitoring therapeutic response in patients with cancer.