Optimizing the geometry of aerodynamic lens injectors for single-particle coherent diffractive imaging of gold nanoparticles

Single-particle X-ray diffractive imaging (SPI) of small (bio-)nanoparticles (NPs) requires optimized injectors to collect sufficient diffraction patterns to allow for the reconstruction of the NP structure with high resolution. Typically, aerodynamic lens-stack injectors are used for NP injection. However, current injectors were developed for larger NPs (>100 nm), and their ability to generate high-density NP beams suffers with decreasing NP size. Here, an aerodynamic lens-stack injector with variable geometry and a geometry-optimization procedure are presented. The optimization for 50 nm gold-NP (AuNP) injection using a numerical-simulation infrastructure capable of calculating the carrier-gas flow and the particle trajectories through the injector is also introduced. The simulations were experimentally validated using spherical AuNPs and sucrose NPs. In addition, the optimized injector was compared with the standard-installation `Uppsala injector' for AuNPs. Results for these heavy particles showed a shift in the particle-beam focus position rather than a change in beam size, which results in a lower gas background for the optimized injector. Optimized aerodynamic lens-stack injectors will allow one to increase NP beam density, reduce the gas background, discover the limits of current injectors and contribute to structure determination of small NPs using SPI.

Quantitative hyperspectral coherent diffractive imaging spectroscopy of a solid-state phase transition in vanadium dioxide

Solid-state systems can host a variety of thermodynamic phases that can be controlled with magnetic fields, strain, or laser excitation. Many phases that are believed to exhibit exotic properties only exist on the nanoscale, coexisting with other phases that make them challenging to study, as measurements require both nanometer spatial resolution and spectroscopic information, which are not easily accessible with traditional x-ray spectromicroscopy techniques. Here, we use coherent diffractive imaging spectroscopy (CDIS) to acquire quantitative hyperspectral images of the prototypical quantum material vanadium oxide across the vanadium L2,3 and oxygen K x-ray absorption edges with nanometer-scale resolution. We extract the full complex refractive indices of the monoclinic insulating and rutile conducting phases of VO2 from a single sample and find no evidence for correlation-driven phase transitions. CDIS will enable quantitative full-field x-ray spectromicroscopy for studying phase separation in time-resolved experiments and other extreme sample environments where other methods cannot operate.

A multipurpose end-station for atomic, molecular and optical sciences and coherent diffractive imaging at ELI beamlines

We report on the status of a users’ end-station, MAC: a Multipurpose station for Atomic, molecular and optical sciences and Coherent diffractive imaging, designed for studies of structure and dynamics of matter in the femtosecond time-domain. MAC is located in the E1 experimental hall on the high harmonic generation (HHG) beamline of the ELI Beamlines facility. The extreme ultraviolet beam from the HHG beamline can be used at the MAC end-station together with a synchronized pump beam (which will cover the NIR/Vis/UV or THz range) for time-resolved experiments on different samples. Sample delivery systems at the MAC end-station include a molecular beam, a source for pure or doped clusters, ultrathin cylindrical or flat liquid jets, and focused beams of substrate-free nanoparticles produced by an electrospray or a gas dynamic virtual nozzle combined with an aerodynamic lens stack. We further present the available detectors: electron/ion time-of-flight and velocity map imaging spectrometers and an X-ray camera, and discuss future upgrades: a magnetic bottle electron spectrometer, production of doped nanodroplets and the planned developments of beam capabilities at the MAC end-station.

Polarimetric coherent diffraction imaging on cancer-associated fibroblasts and SARS-CoV-2 viruses

Simultaneously non-destructive, high resolution, and label-free imaging are of paramount importance for studies of complex biological systems, from viruses to cell cultures. Electron imaging techniques achieve extreme resolution but require slicing the sample to obtain volumetric information. On the other hand, X-rays’ high penetrative ability combined with cryogenic temperatures allows access to high resolution while preserving the sample’s structure. However, both X-ray and electron techniques do not currently allow label-free imaging with tissue specificity. Here, we combine a polarimetric approach with coherent diffractive imaging to reveal new ways to overcome this by mapping variations of anisotropy in the complex refractive index of cellular structures to differentiate between various tissues without chemical labeling. In this article, we demonstrate imaging of cancer-associated fibroblasts using birefringent coherent diffractive imaging with enhanced sensitivity to fibrous structures and their orientation as well as the possibility to differentiate the nucleus of the cell. We also propose a modeled soft X-ray experiment on the SARS-CoV-2 virus to address the possibility of leveraging the polarimetric birefringent contrast to spatially resolve the dynamical interaction of the virus with its host environment. We hope that our approach can open up avenues in the future to map and understand how SARS viruses bind with human epithelial cells.

A wave optics model for the effect of partial coherence on coherent diffractive imaging

With the development of fourth-generation synchrotron sources, coherent diffractive imaging (CDI) will be a mainstream method for 3D structure determination at nanometre resolution. The partial coherence of incident X-rays plays a critical role in the reconstructed image quality. Here a wave optics model is proposed to analyze the effect of partial coherence on CDI for an actual beamline layout, based on the finite size of the source and the influence of the optics on the wavefront. Based on this model, the light field distribution at any plane, the coherence between any two points on this plane and CDI experiments can be simulated. The plane-wave CDI simulation result also shows that in order to reconstruct good image quality of complex samples the visibility of the interference fringes of any two points in the horizontal and vertical directions of the incident light field at the sample needs to be higher than 0.95.