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LED-pump-X-ray-multiprobe crystallography for sub-second timescales.
Hatcher, Lauren E; Warren, Mark R; Skelton, Jonathan M; Pallipurath, Anuradha R; Saunders, Lucy K; Allan, David R; Hathaway, Paul; Crevatin, Giulio; Omar, David; Williams, Ben H; Coulson, Ben A; Wilson, Chick C; Raithby, Paul R.
Afiliación
  • Hatcher LE; Department of Chemistry, University of Bath, Bath, UK.
  • Warren MR; School of Chemistry, Cardiff University, Cardiff, UK.
  • Skelton JM; Diamond Light Source, Harwell Science and Innovation Campus, Didcot, UK.
  • Pallipurath AR; Department of Chemistry, University of Bath, Bath, UK.
  • Saunders LK; Department of Chemistry, University of Manchester, Manchester, UK.
  • Allan DR; Department of Chemistry, University of Bath, Bath, UK.
  • Hathaway P; School of Chemical and Process Engineering, University of Leeds, Leeds, UK.
  • Crevatin G; Diamond Light Source, Harwell Science and Innovation Campus, Didcot, UK.
  • Omar D; Diamond Light Source, Harwell Science and Innovation Campus, Didcot, UK.
  • Williams BH; Diamond Light Source, Harwell Science and Innovation Campus, Didcot, UK.
  • Coulson BA; Diamond Light Source, Harwell Science and Innovation Campus, Didcot, UK.
  • Wilson CC; Diamond Light Source, Harwell Science and Innovation Campus, Didcot, UK.
  • Raithby PR; Diamond Light Source, Harwell Science and Innovation Campus, Didcot, UK.
Commun Chem ; 5(1): 102, 2022 Aug 26.
Article en En | MEDLINE | ID: mdl-36697958
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(Bu4dien)(NO2)][BPh4] 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.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Commun Chem Año: 2022 Tipo del documento: Article Pais de publicación: Reino Unido

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Commun Chem Año: 2022 Tipo del documento: Article Pais de publicación: Reino Unido