Sapnik, Adam F;
Chater, Philip A;
Keeble, Dean S;
Evans, John SO;
Bertolotti, Federica;
Guagliardi, Antonietta;
Støckler, Lise J;
... Keen, David A; + view all
(2025)
High-quality ultra-fast total scattering and pair distribution function data using an X-ray free-electron laser.
IUCrJ
, 12
(5)
10.1107/S205225252500538X.
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Abstract
High-quality total scattering data, a key tool for understanding atomic-scale structure in disordered materials, require stable instrumentation and access to high momentum transfers. This is now routine at dedicated synchrotron instrumentation using high-energy X-ray beams, but it is very challenging to measure a total scattering dataset in less than a few microseconds. This limits their effectiveness for capturing structural changes that occur at the much faster timescales of atomic motion. Current X-ray free-electron lasers (XFELs) provide femtosecond-pulsed X-ray beams with maximum energies of ∼24 keV, giving the potential to measure total scattering and the attendant pair distribution functions (PDFs) on femtosecond timescales. We demonstrate that this potential has been realized using the HED scientific instrument at the European XFEL and present normalized total scattering data for 0.35 Å-1 < Q < 16.6 Å-1 and their PDFs from a broad spectrum of materials, including crystalline, nanocrystalline and amorphous solids, liquids and clusters in solution. We analyzed the data using a variety of methods, including Rietveld refinement, small-box PDF refinement, joint reciprocal-real-space refinement, cluster refinement and Debye scattering analysis. The resolution function of the setup is also characterized. We conclusively show that high-quality data can be obtained from a single ∼30 fs XFEL pulse for multiple different sample types. Our efforts not only significantly increase the existing maximum reported Q range for an S(Q) measured at an XFEL but also mean that XFELs are now a viable X-ray source for the broad community of people using reciprocal-space total scattering and PDF methods in their research.
| Type: | Article |
|---|---|
| Title: | High-quality ultra-fast total scattering and pair distribution function data using an X-ray free-electron laser |
| Location: | England |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1107/S205225252500538X |
| Publisher version: | https://doi.org/10.1107/s205225252500538x |
| Language: | English |
| Additional information: | This is an open-access article distributed under the terms of the Creative Commons Attribution (CC-BY) Licence, which permits unrestricted use, distribution, and reproduction in any medium, provided the original authors and source are cited. |
| Keywords: | XFELs, femtosecond studies, nanocrystals, pair distribution function, pump–probe, time-resolved studies, total scattering |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > London Centre for Nanotechnology |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10212444 |
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