The role of metal ions in X-ray induced photochemistry
arXiv:1505.02079 · doi:10.1038/nchem.2429
Abstract
Metal ions play numerous important roles in biological systems being central to the function of biomolecules. In this letter we show that the absorption of X-rays by these ions leads to a complicated chain of ultrafast relaxation steps resulting in the complete degradation of their nearest environment. We conducted high quality ab initio studies on microsolvated Mg clusters demonstrating that ionisation of an 1s-electron of Mg leads to a complicated electronic cascade comprising both intra- and intermolecular steps and lasting only a few hundreds femtoseconds. The metal cation reverts to its original charge state at the end of the cascade, while the nearest solvation shell becomes multiply ionised and large concentrations of radical and slow electron species build up in the metal vicinity. We conclude that such cascades involving metal ions are essential for understanding the radiation chemistry of solutions and radiation damage to metal containing biomolecules.
Supplementary Material added; Bibliography updated
References in corpus (2)
Cited by in corpus (19)
- Highly efficient double ionization of mixed alkali dimers by intermolecular Coulombic decay
- Interatomic Coulombic decay in helium nanodroplets
- Multi-reference protocol for (auto)ionization spectra: application to molecules
- Absorbed dose evaluation of Auger electron-emitting radionuclides: impact of input decay spectra on dose point kernels and S-values
- Observation and Control of Laser-Enabled Auger Decay
- Multi-reference quantum chemistry protocol for simulating autoionization spectra: Test of ionization continuum models for the neon atom
- Multiscale simulation of the focused electron beam induced deposition process
- Electron transfer mediated decay of alkali dimers attached to He nanodroplets
- Time-resolved study of resonant interatomic Coulombic decay in helium nanodroplets
- Ultrafast intermolecular energy transfer from vibrations to electronic motion
- Time-resolved Ultrafast Interatomic Coulombic Decay in Superexcited Sodium-doped Helium Nanodroplets
- Efficient Indirect Interatomic Coulombic Decay Induced by Photoelectron Impact Excitation in Large He Nanodroplets
- Electron energy loss and angular asymmetry induced by elastic scattering in helium droplets
- Decay Processes in Cationic Alkali Metals in Microsolvated Clusters: A Complex Absorbing Potential Based Equation-of-Motion Coupled Cluster Investigation
- Time-resolved Spectroscopy of Interparticle Coulombic Decay Processes
- Effect of Protonation and Deprotonation on Electron Transfer Mediated Decay and Interatomic Coulombic Decay
- Radiationless decay spectrum of O 1s double core holes in liquid water
- Observation of Nuclear-wavepacket Interference in Ultrafast Inter-atomic Energy Transfer
- Variability in X-ray induced effects in [Rh(COD)Cl]2 with changing experimental parameters