A measurement of the evolution of Interatomic Coulombic Decay in the time domain

During the last 15 years a novel decay mechanism of excited atoms has been discovered and investigated. This so called ''Interatomic Coulombic Decay'' (ICD) involves the chemical environment of the electronically excited atom: the excitation energy is transferred (in many cases over long distances) to a neighbor of the initially excited particle usually ionizing that neighbor. It turned out that ICD is a very common decay route in nature as it occurs across van-der-Waals and hydrogen bonds. The time evolution of ICD is predicted to be highly complex, as its efficiency strongly depends on the distance of the atoms involved and this distance typically changes during the decay. Here we present the first direct measurement of the temporal evolution of ICD using a novel experimental approach.Comment: 6 pages, 4 figures, submitted to PR

Interatomic-Coulombic-decay-induced recapture of photoelectrons in helium dimers

We investigate the onset of photoionization shakeup induced interatomic Coulombic decay (ICD) in He2 at the He+*(n = 2) threshold by detecting two He+ ions in coincidence. We find this threshold to be shifted towards higher energies compared to the same threshold in the monomer. The shifted onset of ion pairs created by ICD is attributed to a recapture of the threshold photoelectron after the emission of the faster ICD electron.Comment: 5 Pages, 2 Figure

Vibrationally Resolved Decay Width of Interatomic Coulombic Decay in HeNe

We investigate the ionization of HeNe from below the He 1s3p excitation to the He ionization threshold. We observe HeNe$^+$ ions with an enhancement by more than a factor of 60 when the He side couples resonantly to the radiation field. These ions are an experimental proof of a two-center resonant photoionization mechanism predicted by Najjari et al. [Phys. Rev. Lett. 105, 153002 (2010)]. Furthermore, our data provide electronic and vibrational state resolved decay widths of interatomic Coulombic decay (ICD) in HeNe dimers. We find that the ICD lifetime strongly increases with increasing vibrational state.Comment: 7 pages, 5 figure

Optimised XUV holography using spatially shaped high harmonic beams

A phase-only spatial light modulator is used to generate multiple infrared foci, the positions and intensities of which can be controlled programmably, allowing the generation and control of multiple high harmonic beams. Using two such high harmonic beams Fourier transform holography is performed with separate illumination of the object and reference pinhole, making optimal use of the available photon flux. This technique provides new opportunities for imaging at extreme ultraviolet wavelengths

Bond-rearrangement and ionization mechanisms in the photo-double-ionization of simple hydrocarbons (C2H4, C2H3F, and 1,1-C2H2F2) near and above threshold

Citation: Gaire, B., Gatton, A., Wiegandt, F., Neff, J., Janke, C., Zeller, S., . . . Weber, T. (2016). Bond-rearrangement and ionization mechanisms in the photo-double-ionization of simple hydrocarbons (C2H4, C2H3F, and 1,1-C2H2F2) near and above threshold. Physical Review A, 94(3), 8. doi:10.1103/PhysRevA.94.033412We investigate bond-rearrangement driven by photo-double-ionization (PDI) near and above the double-ionization threshold in a sequence of carbon-carbon double-bonded hydrocarbon molecules: ethylene, fluoroethylene, and 1,1-difluoroethylene. We employ the kinematically complete cold target recoil ion momentum spectroscopy method to resolve all photo-double-ionization events leading to two-ion fragments. We observe changes in the branching ratios of different dissociative ionization channels depending on the presence of no, one, or two fluorine atoms. The role of the fluorine atom in the bond-rearrangement channels is intriguing, as evident by the reordering of the threshold energies of the PDI in the fluorinated molecules. These effects offer a compelling argument that the electronegativity of the fluorine (or the polarity of the molecule) strongly influences the potential energy surfaces of the molecules and drives bond rearrangement during the dissociation process. The energy sharing and the relative angle between the three-dimensional momentum vectors of the two electrons enable us to distinguish between knockout and other ionization mechanisms of the PDI processes