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A novel ultrahigh-resolution x-ray microscope achieves 8-nm spatial resolution and accurately maps chemistry in nanomaterials., The analysis of chemical states and morphology in nanomaterials is central to many areas of science. We address this need with an ultrahigh-resolution scanning transmission soft x-ray microscope. Our instrument provides multiple analysis tools in a compact assembly and can achieve few-nanometer spatial resolution and high chemical sensitivity via x-ray ptychography and conventional scanning microscopy. A novel scanning mechanism, coupled to advanced x-ray detectors, a high-brightness x-ray source, and high-performance computing for analysis provide a revolutionary step forward in terms of imaging speed and resolution. We present x-ray microscopy with 8-nm full-period spatial resolution and use this capability in conjunction with operando sample environments and cryogenic imaging, which are now routinely available. Our multimodal approach will find wide use across many fields of science and facilitate correlative analysis of materials with other types of probes.

Morphological details of calcium silicate hydrate (C–S–H) stemming from the hydration process of Portland cement (PC) phases are crucial for understanding the PC-based systems but are still only partially known. Here we introduce the first soft X-ray ptychographic imaging of tricalcium silicate (C3S) hydration products. The results are compared using both scanning transmission X-ray and electron transmission microscopy data. The evidence shows that ptychography is a powerful method to visualize the details of outer and inner product C–S–H of fully hydrated C3S, which have fibrillar and an interglobular structure with average void sizes of 20 nm, respectively. The high-resolution ptychrography image enables us to perform morphological quantification of C–S–H, and, for the first time, to possibly distinguish the contributions of inner and outer product C–S–H to the small angle scattering of cement paste. The results indicate that the outer product C–S–H is mainly responsible for the q−3 regime, whereas the inner product C–S–H transitions to a q−2 regime. Various hypotheses are discussed to explain these regimes.

A grand challenge in soft x-ray spectroscopy is to drive the resolving power of monochromators and spectrometers from the 10(4) achieved routinely today to well above 10(5). This need is driven mainly by the requirements of a new technique that is set to have enormous impact in condensed matter physics, Resonant Inelastic X-ray Scattering (RIXS). Unlike x-ray absorption spectroscopy, RIXS is not limited by an energy resolution dictated by the core-hole lifetime in the excitation process. Using much higher resolving power than used for normal x-ray absorption spectroscopy enables access to the energy scale of soft excitations in matter. These excitations such as magnons and phonons drive the collective phenomena seen in correlated electronic materials such as high temperature superconductors. RIXS opens a new path to study these excitations at a level of detail not formerly possible. However, as the process involves resonant excitation at an energy of around 1 keV, and the energy scale of the excitations one would like to see are at the meV level, to fully utilize the technique requires the development of monochromators and spectrometers with one to two orders of magnitude higher energy resolution than has been conventionally possible. Here we investigate the detailed diffraction characteristics of multilayer blazed gratings. These elements offer potentially revolutionary performance as the dispersive element in ultra-high resolution x-ray spectroscopy. In doing so, we have established a roadmap for the complete optimization of the grating design. Traditionally 1st order gratings are used in the soft x-ray region, but we show that as in the optical domain, one can work in very high spectral orders and thus dramatically improve resolution without significant loss in efficiency.

The development of third generation light sources like the Advanced Light Source (ALS) or BESSY II brought to a focus the need for high performance synchrotron optics with unprecedented tolerances for slope error and micro roughness. Proposed beam lines at Free Electron Lasers (FEL) require optical elements up to a length of one meter, characterized by a residual slope error in the range of 0.1murad (rms), and rms values of 0.1 nm for micro roughness. These optical elements must be inspected by highly accurate measuring instruments, providing a measurement uncertainty lower than the specified accuracy of the surface under test. It is essential that metrology devices in use at synchrotron laboratories be precisely characterized and calibrated to achieve this target. In this paper we discuss a proposal for a Universal Test Mirror (UTM) as a realization of a high performance calibration instrument. The instrument would provide an ideal calibration surface to replicate a redundant surface under test of redundant figure. The application of a sophisticated calibration instrument will allow the elimination of the majority of the systematic error from the error budget of an individual measurement of a particular optical element. We present the limitations of existing methods, initial UTM design considerations, possible calibration algorithms, and an estimation of the expected accuracy.

A new strategic plan is in place to upgrade the ALS so it can continue to address fundamental questions, such as size-dependent and dimensional-confinement phenomena at the nanoscale; correlation and complexity in physical, biological, and environmental systems; and temporal evolution, assembly, dynamics and ultrafast phenomena. Moreover, the growing number of ALS users (now exceeding 2,000 per year) requires increased attention. Accordingly, our plan concentrates on projects that will continue to make it possible for ALS users to address grand scientific and technological challenges with incisive world-class tools and quality user support. Our highest priority is to begin top-off operation, in which electrons are injected into the storage ring at intervals of approximately 1 minute. The combination of top-off and concurrent development of small-gap in-vacuum undulators and superconducting undulators will allow an increase in brightness from eight to more than 100 times, depending on the specific undulators and photon energy range. As part of our core mission in the VUV and soft x-ray regions, we plan to exploit these accelerator developments to extend our capabilities for high spatial and temporal resolution and utilize the remarkable coherence properties of the ALS in a new generation of beamlines. Ranked by priority, several proposed beamlines will follow completion of five new beamlines already under construction or funded. The intellectual excitement of the ALS has been a powerful tool in the recruitment and retention of outstanding staff, but additional sustained efforts are required to increase diversity both in gender and in underrepresented groups. To this end, we intend to expand the ALS Doctoral Fellowship Program by giving special emphasis to underrepresented groups. We also envision a distinguished postdoctoral fellowship program with the same emphasis, to increase and diversify our pool of candidates for beamline scientist positions.

A new undulator beam line has been built and commissioned at the Advanced Light Source for illumination of the PEEM3 microscope. The beam line delivers high flux beams over an energy range from C1s through the transition metals to include the M edges of the magnetic rare earth elements. We present details of the optical design, and data on the performance of the zero‐order tracking of the photon energy.

We present examples of the application of synchrotron-based spectroscopies and microscopies to environmentally relevant samples. The experiments were performed at the molecular environmental science beamline (11.0.2) at the Advanced Light Source, Lawrence Berkeley National Laboratory. Examples range from the study of water monolayers on Pt(1 1 1) single crystal surfaces using X-ray emission spectroscopy and the examination of alkali halide solution/water vapor interfaces using ambient pressure photoemission spectroscopy, to the investigation of actinides, river water biofilms, Al-containing colloids and mineral–bacteria suspensions using scanning transmission X-ray spectromicroscopy. The results of our experiments show that spectroscopy and microscopy in the soft X-ray energy range are excellent tools for the investigation of environmentally relevant samples under realistic conditions, i.e., with water or water vapor present at ambient temperature.

The ratio of double to single ionization of He by 85--400 eV photons has been measured using cold target recoil ion momentum spectroscopy. This technique allows the elimination of all possible systematic errors discussed so far in the literature on this subject. We find the ratio in this energy range to be about 25% lower than previously assumed.

The SpectroMicroscopy Facility at the Advanced Light Source is based on a high brightness, high‐resolution beamline, and includes a collection of projects designed to exploit the unique characteristics of the soft x‐ray beam. The beamline itself is comprised of a 5‐m long, 5‐cm‐period undulator, a spherical‐grating monochromator with water‐cooled gratings. Adaptive optics refocus the monochromatic beam to two ‘‘microfocus’’ experimental stations with spot sizes less than 50 μm diameter and a third ‘‘nanofocus’’ station uses a zone‐plate lens to further demagnify the microfocus spot. Experimental stations include an ‘‘ultraESCA’’ spectrometer for small‐area spectroscopy and photoelectron diffraction, a scanning transmission x‐ray microscope, and photoelectron microscopes. Commissioning experiments of microscopic actinide photoemission, surface‐core‐level photoelectron diffraction, and high‐resolution soft x‐ray fluorescence demonstrate dramatic improvements in sensitivity due to the high brightness and sma...