DOI: 10.5281/zenodo.10600583
title: The conception of a solvated electron: X-ray-induced attosecond electron dynamics of aqueous ions - data

description: Data set pertaining to the article "Attosecond formation of charge-transfer-to-solvent states of aqueous ions probed using the core-hole-clock technique", published in Nature Communications.

Here we describe the time-evolution of core level excited electronic states of metal ions in aqueous solution on an ultrashort time scale. Extensive simulations towards this project were carried out. Simulated data include geometries for solvated metal ion complexes and their X-Ray absorption spectra. Experimental data were recorded by photoemission spectroscopy from a liquid jet source using synchrotron radiation. 

Files with extension .h5 are hdf5-files structured according to the NeXus standard v2022.07, seehttps://www.nexusformat.org/https://fairmat-experimental.github.io/nexus-fairmat-proposal/50433d9039b3f33299bab338998acb5335cd8951/mpes-structure.htmlNeXus data files can be opened with any software capable of opening hdf5-structured files. The following viewers are adapted to the specifics of the NeXus data format:* nexpy (distributed with python)* https://h5web.panosc.eu/h5wasm (web-based NeXus viewer maintained by the European Photon and Neutron Open Science Cloud-consortium)

In each NeXus file-entry, two types of spectra are shown:1. Sweep-averaged spectra, integrated over the non-dispersive coordinate of our detector ('data') if applicable.2. As-measured data ('raw').

Files with extension .csv are comma-separated ascii-files, designed to be opened with a spreadsheet programme.

The following files are provided:




Filename
Content


 
Experimental Data:


na_mg_al_1s-resonance_cfs.h5
Series of experimental photoemission spectra recorded over the 1s - val resonances, for NaCl, MgCl2 andAlCl3 metallic salt solutions


 
Theoretical Data:


th.geometries.zip
Cartesian coordinates of the constituents of metal-water clusters containing 6 water molecules and containing 18 water molecules. Unit of length is Ångström.


th.excitation_energy.zip
Excitation energies for metal-water clusters containing 6 water molecules and containing 18 water molecule, at various levels of approximation. tddft-src2: at the SRC2-R2 level with a cc-pCVTZ basis set on the cations and a cc-pVTZ basis set on the water molecules in a polarizable continuum; eomccsd: at the EOM-EE-CCSD level with a cc-pCVTZ basis set on the cations and a cc-pVTZ basis set on the water molecules. For the purpose of spectra construction in Figure 1, each calculated spectral point was broadened by a phenomenological value of 0.2 eV. Energies are in eV, transition dipole moment components in e*bohr.


th.spektrum.pade.zip
Excitation energies for metal-water clusters containing 6 water molecules calculated at the RT-TDDFT level with a cc-pVTZ basis set. For each cation, 3 trajectories were run. Energies are in eV.


th.excitation_energy.zip
Exciton analysis of the wave function (RMS electron size) for a set of 50 geometries of clusters containing 6 water molecules (small) or 18 water molecules (large) calculated at the SRC2-R2/cc-pVTZ level. The oscillator strengths are in a.u., the size of the electron is in Ångström.


description_zenodo.pdf
More detailed description of the theoretical data sets.




If you use part or all of these data in your scientific work we kindly ask you to provide us a copy. Contact: Uwe Hergenhahn, uhe@fhi.mpg.de .
description: Funding Information: Research conducted at MAX IV, a Swedish national user facility, is supported by the Swedish Research Council under contract 2018-07152, the Swedish Governmental Agency for Innovation Systems under contract 2018-04969, and Formas under contract 2019-02496. B.W. and U.H. acknowledge funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme under Grant Agreement No. 883759-AQUACHIRAL. P.S. and E.M. thank the Czech Science Foundation for the support via project number 23-07066S. F.T. acknowledges funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) - Project 509471550, Emmy Noether Programme. F.T. and B.W. acknowledge support by the MaxWater initiative of the Max-Planck-Gesellschaft. C.C. acknowledges the Swedish Research Council (project 2018-00740) and the Helmholtz Association through the Center of Free-Electron Laser Science at DESY. O.B. acknowledges funding from the Swedish Research Council (VR) for the project VR 2023-04346.