LED-pump-X-ray-multiprobe crystallography for sub-second timescales

Paul Raithby, Lauren Hatcher, Mark Warren, Jonathan Skelton, Anuradha R. Pallipurath, Lucy Saunders, David Allan, P Hathaway, G Crevatin, D Omar, B H Williams, Benjamin Coulson, Chick Wilson

Research output: Contribution to journalArticlepeer-review

4 Citations (SciVal)

Abstract

The visualization of chemical processes that occur in the solid-state is key to the design of new functional materials. One of the challenges in these studies is to monitor the processes across a range of timescales in real-time. Here, we present a pump-multiprobe single-crystal X-ray diffraction (SCXRD) technique for studying photoexcited solid-state species with millisecond-to-minute lifetimes. We excite using pulsed LEDs and synchronise to a gated X-ray detector to collect 3D structures with sub-second time resolution while maximising photo-conversion and minimising beam damage. Our implementation provides complete control of the pump-multiprobe sequencing and can access a range of timescales using the same setup. Using LEDs allows variation of the intensity and pulse width and ensures uniform illumination of the crystal, spreading the energy load in time and space. We demonstrate our method by studying the variable-temperature kinetics of photo-activated linkage isomerism in [Pd(Bu 4dien)(NO 2)][BPh 4] single-crystals. We further show that our method extends to following indicative Bragg reflections with a continuous readout Timepix3 detector chip. Our approach is applicable to a range of physical and biological processes that occur on millisecond and slower timescales, which cannot be studied using existing techniques.

Original languageEnglish
Article number102
JournalCommunications Chemistry
Volume5
Issue number1
DOIs
Publication statusPublished - 26 Aug 2022

Bibliographical note

Funding Information:
The authors thank Diamond Light Source for the award of synchrotron beamtime in visits MT17306-1, MT17306-2 and CM19670-3. P.R.R., L.E.H., J.M.S. and A.R.P. are grateful to the EPSRC for support (EP/K004956/1). L.E.H. is currently supported by a Royal Society University Research Fellowship (URF\R1\191104). J.M.S. is currently supported by a UKRI Future Leaders Fellowship (MR/T043121/1) and previously held a University of Manchester Presidential Fellowship.

Funding Information:
The authors thank Diamond Light Source for the award of synchrotron beamtime in visits MT17306-1, MT17306-2 and CM19670-3. P.R.R., L.E.H., J.M.S. and A.R.P. are grateful to the EPSRC for support (EP/K004956/1). L.E.H. is currently supported by a Royal Society University Research Fellowship (URF\R1\191104). J.M.S. is currently supported by a UKRI Future Leaders Fellowship (MR/T043121/1) and previously held a University of Manchester Presidential Fellowship.

Publisher Copyright:
© 2022, The Author(s).

Keywords

  • Time resolved X-ray diffraction
  • LEDs
  • Pump-probe
  • Molecular complex

ASJC Scopus subject areas

  • Chemistry(all)

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