A design of resonant inelastic X-ray scattering (RIXS) spectrometer for spatial- and time-resolved spectroscopy.

The optical design of a Hettrick-Underwood-style soft X-ray spectrometer with Wolter type 1 mirrors is presented. The spectrometer with a nominal length of 3.1 m can achieve a high resolving power (resolving power higher than 10000) in the soft X-ray regime when a small source beam (<3 µm in the grating dispersion direction) and small pixel detector (5 µm effective pixel size) are used. Adding Wolter mirrors to the spectrometer before its dispersive elements can realize the spatial imaging capability, which finds applications in the spectroscopic studies of spatially dependent electronic structures in tandem catalysts, heterostructures, etc. In the pump-probe experiments where the pump beam perturbs the materials followed by the time-delayed probe beam to reveal the transient evolution of electronic structures, the imaging capability of the Wolter mirrors can offer the pixel-equivalent femtosecond time delay between the pump and probe beams when their wavefronts are not collinear. In combination with some special sample handing systems, such as liquid jets and droplets, the imaging capability can also be used to study the time-dependent electronic structure of chemical transformation spanning multiple time domains from microseconds to nanoseconds. The proposed Wolter mirrors can also be adopted to the existing soft X-ray spectrometers that use the Hettrick-Underwood optical scheme, expanding their capabilities in materials research

Ultracold electrons via Near-Threshold Photoemission from Single-Crystal Cu(100)

Achieving a low mean transverse energy or temperature of electrons emitted from the photocathode-based electron sources is critical to the development of next-generation and compact X-ray Free Electron Lasers and Ultrafast Electron Diffraction, Spectroscopy and Microscopy experiments. In this paper, we demonstrate a record low mean transverse energy of 5 meV from the cryo-cooled (100) surface of copper using near-threshold photoemission. Further, we also show that the electron energy spread obtained from such a surface is less than 11.5 meV, making it the smallest energy spread electron source known to date: more than an order of magnitude smaller than any existing photoemission, field emission or thermionic emission based electron source. Our measurements also shed light on the physics of electron emission and show how the energy spread at few meV scale energies is limited by both the temperature and the vacuum density of states

Thermal limit to the intrinsic emittance from metal photocathodes

Measurements of the intrinsic emittance and transverse momentum distributions obtained from a metal (antimony thin film) photocathode near and below the photoemission threshold are presented. Measurements show that the intrinsic emittance is limited by the lattice temperature of the cathode as the incident photon energy approaches the photoemission threshold. A theoretical model to calculate the transverse momentum distributions near this photoemission threshold is presented. An excellent match between the experimental measurements and the theoretical calculations is demonstrated. These measurements are relevant to low emittance electron sources for Free Electron Lasers and Ultrafast Electron Diffraction experiments

Fabrication and characterization of ultra-high resolution multilayer-coated blazed gratings

Multilayer coated blazed gratings with high groove density are the most promising candidate for ultra-high resolution soft x-ray spectroscopy. They combine the ability of blazed gratings to concentrate almost all diffraction energy in a desired high diffraction order with high reflectance soft x-ray multilayers. However in order to realize this potential, the grating fabrication process should provide a near perfect groove profile with an extremely smooth surface of the blazed facets. Here we report on successful fabrication and testing of ultra-dense saw-tooth substrates with 5,000 and 10,000 lines/mm

Fabrication and characterization of a new high density Sc/Si multilayer sliced grating

State of the art soft x-ray spectroscopy techniques like Resonant Inelastic X-ray Scattering (RIXS) require diffraction gratings which can provide extremely high spectral resolution of 105-106. This problem may be addressed with a sliced multilayer grating with an ultra-high groove density (up to 50,000 mm-1) proposed in the recent publication [Voronov, D. L., Cambie, R., Feshchenko, R. M., Gullikson, E., Padmore, H. A., Vinogradov, A. V., Yashchuk, V. V., Proc. SPIE 6705, 67050E (2007)]. It has been suggested to fabricate such a grating by deposition of a soft x-ray multilayer on a substrate which is a blazed saw-tooth grating (echellette) with low groove density. Subsequent polishing applied to the coated grating removes part of the coating and forms an oblique-cut multiline structure that is a sliced multilayer grating. The resulting grating has a short-scale periodicity of lines (bilayers), which is defined by the multilayer period and the oblique-cut angle. We fabricated and tested a Sc/Si multilayer sliced grating suitable for EUV applications, which is a first prototype based on the suggested technique. In order to fabricate an echellette substrate, we used anisotropic KOH etching of a Si wafer. The etching regime was optimized to obtain smooth and flat echellette facets. A Sc/Si multilayer was deposited by dc-magnetron sputtering, and after that it was mechanically polished using a number of diamond pastes. The resulting sliced grating prototype with ~;;270 nm line period has demonstrated a dispersive ability in the 41-49 nm photon wavelength range with a diffraction efficiency of ~;;7percent for the optimized 38th order assigned to the echellette grating of 10 mu m period

Three-dimensional localization of nanoscale battery reactions using soft X-ray tomography.

Battery function is determined by the efficiency and reversibility of the electrochemical phase transformations at solid electrodes. The microscopic tools available to study the chemical states of matter with the required spatial resolution and chemical specificity are intrinsically limited when studying complex architectures by their reliance on two-dimensional projections of thick material. Here, we report the development of soft X-ray ptychographic tomography, which resolves chemical states in three dimensions at 11 nm spatial resolution. We study an ensemble of nano-plates of lithium iron phosphate extracted from a battery electrode at 50% state of charge. Using a set of nanoscale tomograms, we quantify the electrochemical state and resolve phase boundaries throughout the volume of individual nanoparticles. These observations reveal multiple reaction points, intra-particle heterogeneity, and size effects that highlight the importance of multi-dimensional analytical tools in providing novel insight to the design of the next generation of high-performance devices

Ultra-high Resolution Optics for EUV and Soft X-ray Inelastic Scattering

Abstract. We describe a revolutionary new approach to high spectral resolution soft x-ray optics. Conventionally in the soft x-ray energy range, high spectral resolution is obtained by use of a relatively low line density grating operated in 1 st order with small slits. This severely limits throughput. This limitation can be removed by use of a grating either in very high order, or with very high line density, if one can maintain high diffraction efficiency. We have developed a new technology for achieving both of these goals which should allow high throughput spectroscopy, at resolving powers of up to 10 6 at 1 keV. Such optics should provide a revolutionary advance for high resolution lifetime free spectroscopy, such as RIXS, and for pulse compression of chirped beams. We report recent developmental fabrication and characterization of a prototype grating optimized for 14.2 nm EUV light. The prototype grating with a 200 nm period of the blazed grating substrate coated with 20 Mo/Si bilayers with a period of 7.1 nm demonstrates good dispersion in the third order (effective groove density of 15,000 lines per mm) with a diffraction efficiency of more than 33%