This contribution will focus on time-resolved high-energy X-ray scattering pump-probe experiments (EX-ray = 18 keV) conducted at the linear coherent light source (LCLS) with the aim to characterize the position and shape of the wave packets following photoexcitation of the diplatinum anion [Pt2(P2O5H2)4]4- in solution. Photoinduced changes in the electronic structure of the PtPOP molecule lead to a shortening of the Pt-Pt equilibrium distance causing a wave packet oscillation of the Pt-Pt stretch vibration with a period of 224 fs and a decay time of 1 to 2 ps. To simulate the effect of the wave packet dynamics on the difference scattering signal, a model taking into account the evolution of the Pt-Pt distance distribution has been developed and integrated into data analysis. Simulations of difference scattering signals for different distributions of excited-state Pt-Pt distances suggest that a characterization of the position and shape of the wave packet dynamics is predominantly accessible in the high Q range. The data shown in Figure 2 was acquired in collaboration with A. Natan and K. Gaffney, SLAC.

Time-resolved X-ray solution scattering - direct tracking of wave packet dynamics following photoexcitation of the diplatinum complex Pt2(POP)4

ACS Spring 2022

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