Ultrafast Structural Dynamics of Photo-Reactions Revealed by Model-Independent X-ray Cross-Correlation Analysis

Abstract

We applied angular X-ray Cross-Correlation analysis (XCCA) to scattering images from a femtosecond resolution LCLS X-ray free-electron laser (XFEL) pump-probe experiment with solvated PtPOP ([Pt${}_2$(P${}_2$O${}_5$H${}_2$)${}_4$]${}^{4-}$) metal complex molecules. The molecules were pumped with linear polarized laser pulses creating an excited state population with a preferred orientational (alignment) direction. Two time scales of $1.9\pm 1.5$ ps and $46\pm 10$ ps were revealed by model-independent XCCA, associated with an internal structural changes and rotational dephasing, respectively. Our studies illustrate the potential of XCCA to reveal hidden structural information in a model independent analysis of time evolution of solvated metal complex molecules.

8 pages, 5 figures, 50 references