Transient Structures and Kinetics of the Ferrioxalate Redox Reaction Studied by Time-Resolved EXAFS, Optical Spectroscopy, and DFT

Abstract
The photoredox reaction transients of ferrioxalate in water have been studied by means of time-resolved EXAFS and ultrafast optical transient spectroscopy. The transient spectra and kinetics have been measured from the femtosecond to millisecond range, and the Fe−O bond lengths of the ferrioxalate redox reaction transients have been determined with 2 ps time resolution and 0.04 Å accuracy. These data in conjunction with quantum-chemistry DFT and UHF calculations were used to formulate a mechanism for the Fe(III) to Fe(II) redox reaction where dissociation precedes electron transfer. In addition, radical scavenging experiments support the mechanism proposed.