Single particle imaging at x-ray free electron lasers (XFELs) has the potential to determine the structure and dynamics of single biomolecules at room temperature. Two major hurdles have prevented this potential from being reached, namely, the collection of sufficient high-quality diffraction patterns and robust computational purification to overcome structural heterogeneity. We report the breaking of both of these barriers using gold nanoparticle test samples, recording around 10 million diffraction patterns at the European XFEL and structurally and orientationally sorting the patterns to obtain better than 3-nm-resolution 3D reconstructions for each of four samples. With these new developments, integrating advancements in x-ray sources, fast-framing detectors, efficient sample delivery, and data analysis algorithms, we illuminate the path towards sub-nano meter biomolecular imaging. The methods developed here can also be extended to characterize ensembles that are inherently diverse to obtain their full structural landscape. Published by The Optical Society under the terms of the Creative Commons Attribution 4.0 License.
Coherent multi-spectral extreme ultraviolet beams have great potential for providing high spatial and temporal resolution for microscopy and spectroscopy applications. But due to the limitations of short-wavelength optics and the broad bandwidth, it remains a challenge to perform quantitative, high-resolution beam characterization. Here we present a wavefront sensing solution based on multiplexed ptychography, with which we show spectrally resolved, high-resolution beam reconstructions. Furthermore, using these high-fidelity quantitative wavefront measurements, we investigate aberration transfer mechanisms in the high-harmonic-generation process, where we present and explain harmonic-order-dependent astigmatism inheritance from the fundamental wavefront. This ptychographic wavefront sensing concept thus enables detailed studies of the high-harmonic-generation process, such as spatiotemporal effects in attosecond pulse formation.
In recent years, femtosecond extreme-ultraviolet (XUV) and x-ray pulses from free-electron lasers have developed into important probes to monitor processes and dynamics in matter on femtosecond-time and angstrom-length scales. With the rapid progress of versatile ultrafast x-ray spectroscopy techniques and more sophisticated data analysis tools, accurate single-pulse information on the arrival time, duration, and shape of the probing x-ray and XUV pulses becomes essential. Here, we demonstrate that XUV pulses can be converted into terahertz electromagnetic pulses using a spintronic terahertz emitter. We observe that the duration, arrival time, and energy of each individual XUV pulse is encoded in the waveform of the associated terahertz pulses, and thus can be readily deduced from single-shot terahertz time-domain detection.