Resolving structures of transition metal complex reaction intermediates with femtosecond EXAFS

Alexander Britz; Baxter Abraham; Elisa Biasin; Tim Brandt van Driel; Alessandro Gallo; Angel T. Garcia-Esparza; James Glownia; Anton Loukianov; Silke Nelson; Marco Reinhard; Dimosthenis Sokaras; Roberto Alonso-Mori

doi:10.1039/C9CP03483H

Resolving structures of transition metal complex reaction intermediates with femtosecond EXAFS†

Alexander Britz,

*^ab Baxter Abraham,^bc Elisa Biasin,^a Tim Brandt van Driel,^b Alessandro Gallo,^de Angel T. Garcia-Esparza,

^c James Glownia,^b Anton Loukianov,^b Silke Nelson,^b Marco Reinhard,^a Dimosthenis Sokaras*^c and Roberto Alonso-Mori*^b

Author affiliations

* Corresponding authors

^a Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA
E-mail: abritz@slac.stanford.edu

^b Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA
E-mail: robertoa@slac.stanford.edu

^c Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA
E-mail: dsokaras@slac.stanford.edu

^d SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA 94305, USA

^e SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA

Abstract

Femtosecond-resolved Extended X-ray Absorption Fine Structure (EXAFS) measurements of solvated transition metal complexes are successfully implemented at the X-ray Free Electron Laser LCLS. Benchmark experiments on [Fe(terpy)₂]²⁺ in solution show a signal-to-noise ratio on the order of 500, comparable to typical 100 ps-resolution synchrotron measurements. In the few femtoseconds after photoexcitation, we observe the EXAFS fingerprints of a short-lived (∼100 fs) intermediate as well as those of a vibrationally hot long-lived (∼ns) excited state.

This article is part of the themed collection: XFELs: cutting edge X-ray light for chemical and material sciences

Physical Chemistry Chemical Physics

Resolving structures of transition metal complex reaction intermediates with femtosecond EXAFS†

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Resolving structures of transition metal complex reaction intermediates with femtosecond EXAFS

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