Time-resolved studies of interatomic Coulombic decay

Frühling, Ulrike; Trinter, Florian; Karimi, F; Williams, Joshua; Jahnke, T.

doi:10.1016/j.elspec.2015.06.012

Cited by 21 publications

(21 citation statements)

References 68 publications

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“…It is probable that in contrast to most of previous studies of correlated electron dynamics91011125152535455 the precursors for observed CED-channels are populated few picoseconds after the absorption of XUV-photons. On this time-scale the clusters are substantially expanded and resemble a strongly diluted plasma2443.…”

Section: Discussionmentioning

confidence: 62%

“…and since then has been subjected to extensive theoretical and experimental investigations (see e.g. refs 9, 10, 11, 12 for reviews). For instance, low-energy ICD-electrons produced upon ionization of water dimers13 and water clusters14 are considered as a source for radiation damage in biological matter.…”

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confidence: 99%

“…In most previous studies, precursors for ICD or other autoionizing channels are populated directly through resonant or nonresonant absorption of extreme ultraviolet (XUV) photons by individual atoms within a molecule, dimer, or larger cluster9101112. In the X-ray photon energy range a release of the inner-shell electron may cause a collective excitation of valence electrons (shake-up) or release of the outer valence electron (shake-off).…”

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confidence: 99%

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Correlated electronic decay in expanding clusters triggered by intense XUV pulses from a Free-Electron-Laser

Oelze

Schütte

Müller

et al. 2017

Sci Rep

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Irradiation of nanoscale clusters and large molecules with intense laser pulses transforms them into highly-excited non- equilibrium states. The dynamics of intense laser-cluster interaction is encoded in electron kinetic energy spectra, which contain signatures of direct photoelectron emission as well as emission of thermalized nanoplasma electrons. In this work we report on a so far not observed spectrally narrow bound state signature in the electron kinetic energy spectra from mixed Xe core - Ar shell clusters ionized by intense extreme-ultraviolet (XUV) pulses from a free-electron-laser. This signature is attributed to the correlated electronic decay (CED) process, in which an excited atom relaxes and the excess energy is used to ionize the same or another excited atom or a nanoplasma electron. By applying the terahertz field streaking principle we demonstrate that CED-electrons are emitted at least a few picoseconds after the ionizing XUV pulse has ended. Following the recent finding of CED in clusters ionized by intense near-infrared laser pulses, our observation of CED in the XUV range suggests that this process is of general relevance for the relaxation dynamics in laser produced nanoplasmas.

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Section: Discussionmentioning

confidence: 62%

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confidence: 99%

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confidence: 99%

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Correlated electronic decay in expanding clusters triggered by intense XUV pulses from a Free-Electron-Laser

Oelze

Schütte

Müller

et al. 2017

Sci Rep

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“…The superexchange ICD mechanism may be observed experimentally by comparing time-resolved experiments, such as in Refs. [7,32], on Ne clusters doped with an increasing number of He atoms, on the one hand, and on homogeneous Ne clusters, on the other hand. Since these experiments rely on the detection of ions, it might be preferable to use small clusters in order to avoid charge transfer processes following ICD.…”

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confidence: 99%

Interatomic Coulombic Decay Mediated by Ultrafast Superexchange Energy Transfer

et al. 2017

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Inner-valence ionized states of atoms and molecules live shorter if these species are embedded in an environment due to the possibility for ultrafast deexcitation known as interatomic Coulombic decay (ICD). In this Letter we show that the lifetime of these ICD active states decreases further when a bridge atom is in proximity to the two interacting monomers. This novel mechanism, termed superexchange ICD, is an electronic correlation effect driven by the efficient energy transfer via virtual states of the bridge atom. The superexchange ICD is discussed in detail on the example of the NeHeNe trimer. We demonstrate that the decay width of the Ne^{+}(2s^{-1}) ^{2}Σ_{g}^{+} resonance increases 6 times in the presence of the He atom at a distance of 4 Å between the two Ne atoms. Using a simple model, we provide a qualitative explanation of the superexchange ICD and we derive analytical expressions for the dependence of the decay width on the distance between the neon atoms.

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“…Depending on the system, ICD takes place on the femtosecond to picosecond timescales and it is generally the dominant decay pathway unless local Auger decay is operative. While this general characteristic of ICD is well established [7], computing accurately the lifetime of the excited species, or turning from time to energy domain, the energy width of the corresponding state, remains challenging. Several methods have been implemented to compute ab initio ICD widths of ionized and/or excited atoms and molecules in small clusters.…”

Section: Introductionmentioning

confidence: 99%

On the computations of interatomic Coulombic decay widths with R-matrix method

Sisourat

Engin

Gorfinkiel

et al. 2017

The Journal of Chemical Physics

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Interatomic Coulombic Decay (ICD) is a general mechanism in which an excited atom can transfer its excess energy to a neighbor which is thus ionized. ICD belongs to the family of Feshbach resonance processes, and, as such, states undergoing ICD are characterized by their energy width. In this work, we investigate the computations of ICD widths using the R-matrix method as implemented in the UKRmol package. Helium dimer is used here as a benchmark system. The results are compared with those obtained with the well established Fano-Algebraic Diagrammatic Construction method. It is shown that the R-matrix method in its present implementation provides accurate total and partial widths if the kinetic energy of the ICD electron is lower than 10 eV. Advantages and limitations of the R-matrix method on the computations of ICD widths are discussed.

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Time-resolved studies of interatomic Coulombic decay

Cited by 21 publications

References 68 publications

Correlated electronic decay in expanding clusters triggered by intense XUV pulses from a Free-Electron-Laser

Correlated electronic decay in expanding clusters triggered by intense XUV pulses from a Free-Electron-Laser

Interatomic Coulombic Decay Mediated by Ultrafast Superexchange Energy Transfer

On the computations of interatomic Coulombic decay widths with R-matrix method

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