Water Solvent Reorganization upon Ultrafast Resonant Stimulated X‑ray Raman Excitation of a Metalloporphyrin Dimer

Abstract We propose an X-ray Raman pump - X-ray diffraction probe scheme to follow solvation dynamics upon charge migration in a solute molecule. The X-ray Raman pump selectively prepares a valence electronic wavepacket in the solute, while the probe provides information on the entire molecular ensemble. A combination of Molecular Dynamics (MD) and ab initio quantum chemistry simulations is applied to a Zn-Ni porphyrin dimer in water. Using time-resolved X-ray diffraction and pair distribution functions, solvation shell dynamics are extracted. Datasets for the plots data_rdf: Contains RDF data in netcdf4 (readable by xarray) and averaged CSV files. data_sfac: Contains scattering data in netcdf4 (readable by xarray) and averaged CSV files. data_ener: Contains CP2K energy file data for all reference and production runs. data_cdf: Contains csv data files for cumulative distribution function. data_sdf: Contains the cubes files for spatial distribution function. python_codes: Contains python code snippets for recreating figures from the above datasets.