The conception of a solvated electron: X-ray-induced attosecond electron dynamics of aqueous ions - data

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 or .txt 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

SI-Fig6.zip
Ascii representation of the data and fit curves used to determine in 1s lifetime broadening, shown in Fig. 6 of the Supplementary Information.

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.

Version historyv2: fixed incorrect choice of data file for Na scan. Data for lifetime-figure in SI added.v1: initial upload

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, [e-mail] .