title: Microsecond time-resolved energy-dispersive EXAFS measurement and its application to film the thermolysis of (NH₄)₂[PtCl₆].
abstract: Microsecond (μs) time-resolved extended X-ray absorption fine structure spectroscopy (EXAFS) has been developed using an energy-dispersive EXAFS (EDE) setup equipped with a silicon Quantum Detector ULTRA. The feasibility was investigated with a prototypical thermally driven redox reaction, the thermal decomposition of (NH₄)₂[PtCl₆]. EXAFS data were collected with snapshots every 60 μs during the course of the thermolysis reaction, then averaged for 100 times along the reaction to get better signal to noise ratio which reduces the time resolution to 6 millisecond (ms). Our results provide direct structural evidence of cis-PtCl₂(NH₃)₂ as the intermediate, together with continuous electronic and geometric structure dynamics of the reactant, intermediate and final product during the course of the thermolysis of ((NH₄)₂[PtCl₆]. The thermal effect on EXAFS signals at high temperatures is considered in the data analysis, which is essential to follow the reaction process correctly. This method could also be applied to other reaction dynamics.
authors.affiliation: Synchrotron SOLEIL, L'Orme des Merisiers Saint-Aubin, BP 48 91192 Gif sur Yvette Cedex, France. kong@synchrotron-soleil.fr
authors.forename: Qingyu
authors.initials: Q
authors.lastname: Kong
authors.forename: Francois
authors.initials: F
authors.lastname: Baudelet
authors.forename: Jun
authors.initials: J
authors.lastname: Han
authors.forename: Sebastien
authors.initials: S
authors.lastname: Chagnot
authors.forename: Laurent
authors.initials: L
authors.lastname: Barthe
authors.forename: Jon
authors.initials: J
authors.lastname: Headspith
authors.forename: Roger
authors.initials: R
authors.lastname: Goldsbrough
authors.forename: Frederic E
authors.initials: FE
authors.lastname: Picca
authors.forename: Olivier
authors.initials: O
authors.lastname: Spalla