2009/05/07 by Grigory Smolentsev, G. Smolentsev, Gemma Guilera +6 · 7 citations
Physics and Astronomy · Materials Science · #X-ray Spectroscopy and Fluorescence Analysis #Advanced Chemical Physics Studies #Machine Learning in Materials Science
paper · doi:10.1063/1.3125940
A method for the analysis of time-resolved x-ray absorption near edge structure (XANES) spectra is proposed. It combines principal component analysis of the series of experimental spectra, multidimensional interpolation of theoretical XANES as a function of structural parameters, and ab initio XANES calculations. It allows to determine the values of structural parameters for intermediates of chemical reactions and the concentrations of different states as a function of time. This approach is tested using numerically generated data and its possibilities and limitations are discussed. The application of this method to a reaction with methylrhenium trioxide catalyst in solution, for which experimental data were measured using stopped-flow energy-dispersive x-ray absorption spectroscopy technique, is demonstrated. Possibilities and limitations of this experimental technique are also discussed.