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High-quality ultra-fast total scattering and pair distribution function data using an X-ray free electron laser

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. Here, we show that this potential has been realised using the HED scientific instrument at the European XFEL and present normalised total scattering data for 0.35Å−1 < Q < 16.6Å−1 and their PDFs from a broad spectrum of materials, including crystalline, nanocrystalline and amorphous solids, liquids, and clusters in solution. We analyse 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 characterised. 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.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1107/S205225252500538X

Authors


More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Inorganic Chemistry
Role:
Author
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Inorganic Chemistry
Oxford college:
St Anne's College
Role:
Author
ORCID:
0000-0001-9231-3749


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Funder identifier:
https://ror.org/0439y7842
Grant:
EP/W017091/1


Publisher:
International Union of Crystallography
Journal:
IUCrJ More from this journal
Volume:
12
Issue:
5
Article number:
12
Publication date:
2025-07-22
Acceptance date:
2025-06-13
DOI:
EISSN:
2052-2525


Language:
English
Keywords:
Pubs id:
2130324
Local pid:
pubs:2130324
Deposit date:
2025-06-16

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