Resonant interatomic Coulombic decay in HeNe: Electron angular emission distributions

Mhamdi, A.; Trinter, Florian; Rauch, Christian; Weller, M.; Rist, J.; Waitz, M.; Siebert, Juliane; Metz, D.; Jänke, Christian; Kastirke, Gregor; Wiegandt, Florian; Bauer, Tobias; Tia, Maurice; Miranda, Barbara Cunha de; Pitzer, M.; Sann, H.; Schiwietz, G.; Schöffler, M. S.; Simon, M.; Gokhberg, Kirill; Dørner, R.; Jahnke, T.; Demekhin, Ph. V.

doi:10.1103/physreva.97.053407

Cited by 25 publications

(27 citation statements)

References 45 publications

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“…In addition to the correct treatment of the electronic continuum, proper continuum functions also provide angular distributions of ICD electrons. 107 Efficient implementations of post-HF methods are however usually based on square-integrable Gaussian-type functions, which produce only a discrete pseudocontinuum exhibiting the wrong normalization. Nevertheless, these states can be used to compute accurate bound-to-continuum transition moments, for which the long-range behavior of the continuum wave function is irrelevant.…”

Section: Theoretical Approachesmentioning

confidence: 99%

Interatomic and Intermolecular Coulombic Decay

et al. 2020

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Interatomic or intermolecular Coulombic decay (ICD) is a nonlocal electronic decay mechanism occurring in weakly bound matter. In an ICD process, energy released by electronic relaxation of an excited atom or molecule leads to ionization of a neighboring one via Coulombic electron interactions. ICD has been predicted theoretically in the mid nineties of the last century, and its existence has been confirmed experimentally approximately ten years later. Since then, a number of fundamental and applied aspects have been studied in this quickly growing field of research. This review provides an introduction to ICD and draws the connection to related energy transfer and ionization processes. The theoretical approaches for the description of ICD as well as the experimental techniques developed and employed for its investigation are described. The existing body of literature on experimental and theoretical studies of ICD processes in different atomic and molecular systems is reviewed.

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Section: Theoretical Approachesmentioning

confidence: 99%

Interatomic and Intermolecular Coulombic Decay

et al. 2020

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“…Importantly, low energy electrons are typically emitted as a result of the interatomic (or intermolecular) decay process [18][19][20]. It has been demonstrated, that ICD can occur after a manifold of different excitation schemes.Of specific interest in the present context is the socalled resonant interatomic Coulombic decay (RICD) [21][22][23][24][25][26][27][28][29]. In neon dimers, for example, an inner-valence Rydberg excitation (Ne * (2s −1 np)Ne) can decay via the following three competing mechanisms [24]: (i) by autoionization (AI) of the Rydberg state, which is a purely atomic decay ionizing the initially exited site of the arXiv:1810.07415v1 [physics.atm-clus]…”

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confidence: 99%

“…Of specific interest in the present context is the socalled resonant interatomic Coulombic decay (RICD) [21][22][23][24][25][26][27][28][29]. In neon dimers, for example, an inner-valence Rydberg excitation (Ne * (2s −1 np)Ne) can decay via the following three competing mechanisms [24]: (i) by autoionization (AI) of the Rydberg state, which is a purely atomic decay ionizing the initially exited site of the dimer; (ii) by participator resonant ICD (pRICD), in which the np Rydberg electron fills the 2s hole on the same site and the relaxation energy, transferred to the neighbor, is sufficient to ionize a 2p electron (i.e., the opposite site of the dimer becomes ionized in pRICD); and, finally, (iii) by spectator resonant ICD (sRICD), where the ICD process takes place in the presence of the excited Rydberg electron and where the initially excited atom remains excited and the opposite site becomes ionized.…”

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confidence: 99%

“…In order to make a first estimate of the magnitude of the proposed effect, we have examined the sRICD process (1) theoretically. Our calculations were performed employing the stationary Single Center (SC) method and code [30,31], which already provided an accurate description of angular resolved photoionization and decay spectra of diatomic molecules [32][33][34] and weakly bound dimers [29,35] in the past. The transition amplitudes were computed within the frozen core Hartree-Fock approximation at different internuclear distances.…”

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confidence: 99%

“…In order to model this situation theoretically, we have computed the wave functions of the excited 5pσ g/u and 5pπ g/u Rydberg electrons, as described in our previous works [29,[38][39][40][41]. The calculations were performed by employing the SC method at the equilibrium internuclear distance of 3.1Å using the potentials generated by the inner-valence ionized states 2σ −1 g/u .…”

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Breakdown of the Spectator Concept in Low-Electron-Energy Resonant Decay Processes

et al. 2018

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We suggest that low energy electrons, released by resonant decay processes, experience substantial scattering on the electron density of excited electrons, which remain a spectator during the decay. As a result, the angular emission distribution is altered significantly. This effect is expected to be a common feature of low energy secondary electron emission. In this letter, we exemplify our idea by examining the spectator resonant interatomic Coulombic decay (sRICD) of Ne dimers. Our theoretical predictions are confirmed by a corresponding coincidence experiment. 32.80.Hd, 33.60.+q The emission of secondary electrons after ionization or excitation of atoms and molecules has been vastly investigated since its discovery in 1905 by Pierre Auger. Such electronic decay processes provide unique information on electron-electron (configuration) interaction effects in matter. Auger decays can be grouped into two classes: so-called participator decays are cases, where the initially excited electron is actively participating in the decay by either being emitted or being the electron that fills a vacancy in an inner shell. In contrast, in spectator decays the initially excited electron does not participate in the decay but remains in its excited state acting simply as a spectator to the decay. It is commonly accepted that an electronic decay of an ionized or excited atom or molecule can be described in good approximation independently of the initial excitation step. As a consequence, for instance, an electron emitted by an Auger decay after photoionization, does not depend on the polarization properties of the absorbed photon [1]. This approximation is commonly known as the two-step model [2]. For a resonant Auger decay [3,4], this approximation is particularly valid if the excited electron is only witnessing the decay process as a spectator. However, several works have shown, that in special cases, the twostep approximation can break down [5][6][7][8].In the present article we discuss a scenario of a breakdown of the two-step model which is not connected to specific, rare cases in nature, but is expected to occur very generally as soon as the electron emitted by the decay is of low kinetic energy. In this case, the Coulomb repulsion between the outgoing free electron and the excited bound electron may influence the emission direction of the former. Accordingly, for low energy electrons even a spectator electron is expected to influence the emission dynamics, as the wave packet of the slow secondary electron will be scattered by the density of that spectator electron when escaping the system. Such final-state scattering effects, in general, should depend on the spatial symmetry of the excited electron, and information on the polarization of the exciting photon, which is imprinted in the symmetry of the spectator electron, is (in contrast to expectations from the two-step model) transferred to the secondary electron. Please note, that the effect discussed here is very different from the so-called post collision interacti...

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Inter-Coulombic Decay in Laterally Arranged Quantum Dots Controlled by Polarized Lasers

2019

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The inter-Coulombic decay (ICD) process, where one electronically-excited species relaxes, while the neighboring one is concomitantly ionized, is recently discovered likewise in atomic, molecular, biological, and nanostructured systems. Any theoretical prediction of it relies strongly on an accurate treatment of the involved resonance and continuum states. Here, we describe laser-induced ICD in quantum dots with electron dynamics at a multiconfiguration time-dependent Hartree-Fock level for the first time for a two-dimensional continuum, which was possible by implementing an efficient Multigrid POTFIT representation of the Coulomb interaction, such that ICD control with laser polarization is within reach. Conclusively, ICD turns out to be much faster in laterally-arranged self-assembled or lithographic quantum dots connected to a twodimensional wetting-layer continuum than in previously investigated dots in nanowires.

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Resonant interatomic Coulombic decay in HeNe: Electron angular emission distributions

Cited by 25 publications

References 45 publications

Interatomic and Intermolecular Coulombic Decay

Interatomic and Intermolecular Coulombic Decay

Breakdown of the Spectator Concept in Low-Electron-Energy Resonant Decay Processes

Inter-Coulombic Decay in Laterally Arranged Quantum Dots Controlled by Polarized Lasers

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