An assessment of the resolution limitation due to radiation-damage in x-ray diffraction microscopy

X-ray diffraction microscopy (XDM) is a new form of x-ray imaging that is being practiced at several third-generation synchrotron-radiation x-ray facilities. Although only five years have elapsed since the technique was first introduced, it has made rapid progress in demonstrating high-resolution threedimensional imaging and promises few-nm resolution with much larger samples than can be imaged in the transmission electron microscope. Both life- and materials-science applications of XDM are intended, and it is expected that the principal limitation to resolution will be radiation damage for life science and the coherent power of available x-ray sources for material science. In this paper we address the question of the role of radiation damage. We use a statistical analysis based on the so-called "dose fractionation theorem" of Hegerl and Hoppe to calculate the dose needed to make an image of a lifescience sample by XDM with a given resolution. We conclude that the needed dose scales with the inverse fourth power of the resolution and present experimental evidence to support this finding. To determine the maximum tolerable dose we have assembled a number of data taken from the literature plus some measurements of our own which cover ranges of resolution that are not well covered by reports in the literature. The tentative conclusion of this study is that XDM should be able to image frozen-hydrated protein samples at a resolution of about 10 nm with "Rose-criterion" image quality.Comment: 9 pages, 4 figure

The Equilibria of Lipid–K+ Ions in Monolayer at the Air/Water Interface

The effect of K+ ion interaction with monolayers of phosphatidylcholine (lecithin, PC) or cholesterol (Ch) was investigated at the air/water interface. We present surface tension measurements of lipid monolayers obtained using a Langmuir method as a function of K+ ion concentration. Measurements were carried out at 22°C using a Teflon trough and a Nima 9000 tensiometer. Interactions between lecithin and K+ ions or Ch and K+ ions result in significant deviations from the additivity rule. An equilibrium theory to describe the behavior of monolayer components at the air/water interface was developed in order to obtain the stability constants and area occupied by one molecule of lipid–K+ ion complex (LK+). The stability constants for lecithin–K+ ion (PCK+) complex, \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$K_{{{\text{PCK}}^{ + } }} = { 3}. 2 6\times 10^{ 2} {\text{dm}}^{ 3} \,{\text{mol}}^{ - 1}$$\end{document}, and for cholesterol–K+ ion (ChK+) complex, \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$K_{{{\text{ChK}}^{ + } }} = { 1}.00 \times 10^{ 3} {\text{dm}}^{ 3} \,{\text{mol}}^{ - 1}$$\end{document}, were calculated by inserting the experimental data. The value of area occupied by one PCK+ complex is 60 Å2 molecule−1, while the area occupied by one ChK+ complex is 40.9 Å2 molecule−1. The complex formation energy (Gibbs free energy) values for the PCK+ and ChK+ complexes are −14.18 ± 0.71 and −16.92 ± 0.85 kJ mol−1, respectively

Pressure-induced changes in the electronic structure of americium metal

We have conducted electronic-structure calculations for Am metal under pressure to investigate the behavior of the 5f-electron states. Density-functional theory (DFT) does not reproduce the experimental photoemission spectra for the ground-state phase where the 5f electrons are localized, but the theory is expected to be correct when 5f delocalization occurs under pressure. The DFT prediction is that peak structures of the 5f valence band will merge closer to the Fermi level during compression indicating presence of itinerant 5f electrons. Existence of such 5f bands is argued to be a prerequisite for the phase transitions, particularly to the primitive orthorhombic AmIV phase, but does not agree with modern dynamical-mean-field theory (DMFT) results. Our DFT model further suggests insignificant changes of the 5f valence under pressure in agreement with recent resonant x-ray emission spectroscopy, but in contradiction to the DMFT predictions. The influence of pressure on the 5f valency in the actinides is discussed and is shown to depend in a non-trivial fashion on 5f band position and occupation relative to the spd valence bands

X-ray diffraction evidence of ordering in a normal liquid near the solid-liquid interface

We have seen X-ray diffraction peaks establishing that the structure of normal liquids at solid-liquid interfaces is significantly different from the bulk structures. Wetting film thicknesses of ~5000 Å were formed on silicon (111) surfaces with native oxide by pouring and draining the pure liquids; such films are thin enough for X-rays to penetrate easily, but thick enough to eliminate undesired fringes corresponding to the film thickness. The liquids studied were tetrakis(2-ethylhexoxy)silane (TEHOS) and tetrakis(trimethylsiloxy)silane (TTMSS). The observed diffraction peaks are in the specular direction, showing that the liquid molecules form layers parallel to the interface. The layer spacings are comparable to the molecular dimensions, and the peak widths indicate that there are 3–6 layers

pH-dependent kinetics of MgCl2MgCl_2 adsorption under a fatty acid monolayer

International audienceThe effect of subphase pH (5.5 and 10.5) on the structure of behenic-acid monolayers was investigated during Mg2+ adsorption by means of Grazing Incidence X-ray Diffraction (GIXD) and Brewster Angle Microscopy (BAM). The final phase corresponding to an ion superlattice commensurate to the behenic-acid cell is pH-independent. In contrast, the sequence of phases evidenced from the initial L-2-phase to this final state presents at pH 10.5 an additional stage associated to a film condensation toward the L'(2)-phase. The structures of the intermediate states preceding the superstructure nucleation are slightly different, both with a short-range fatty-acid order. Finally, a laser light effect that could result from visible light absorption by the inorganic complexes is evidenced in the final state as well as in the intermediate phases

Evolution toward the X phase of fatty acid Langmuir monolayers on a divalent cation solution

International audienceThe structure of docosanoic acid monolayers spread over chloride salt solutions of copper was investigated by means of isotherm measurements, grazing incidence X-ray diffraction, and Brewster angle microscopy, as a function of the ion concentration and at two subphase pHs (5.5 and 7.5). The X phase is evidenced immediately above a concentration threshold which depends on the pH. The sequence of phases leading to this rigid phase involves two different processes depending oil the pH. The initial L(2h), phase evolves toward an X-like phase through a phase transition which is first order at pH 7.5 while it is second order at pH 5.5. The transition is then followed by a continuous evolution toward the X phase

Transverse correlations and plasticity in the CDW conductor NbSe3_{3} studied by X-ray microbeam diffraction

In whisker-like samples of the quasi-1D conductor NbSe$_{3}$, the presence of longitudinal steps causes shearing of the CDW, and leads to a loss of transverse correlations. We use a microdiffraction setup with a spatial resolution of 300 nm and an angular sensitivity of 5 mdeg to image the resulting CDW contrast between thick and thin portions of the sample. Microdiffraction in the b* - c* plane shows that depinning on the thick, weakly pinned side is accompanied by the loss of diffraction intensity, demonstrating a loss of correlations in qualitative agreement with previous X-ray diffraction topography measurements$^{1}$, but with an order-of-magnitude improvement in spatial resolution. Microdiffraction images in the a* - b* plane reveal a sharp increase in the full width at half maximum in an approximately 1 micron thick region near the step edge and a rotation of the CDW wavevector that varies with applied field. We use the extremal value of the CDW wavevector rotation to estimate the shear modulus of this electronic crystal