Interatomic Coulombic decay widths of helium trimer: A diatomics-in-molecules approach

Sisourat, Nicolas; Kazandjian, Sévan; Randimbiarisolo, Aurélie; Kolorenč, Přemysl

doi:10.1063/1.4942483

Cited by 4 publications

(8 citation statements)

References 59 publications

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“…When ICD takes place in He droplets, the primary process is likely to occur between the ionized atom He + * and arXiv:1707.06902v1 [physics.atm-clus] 21 Jul 2017 its nearest neighbor due to the steep dependence of the ICD rate on interatomic distance [3]. Three-body effects and more complex interactions give only small contributions [21]. However, in He droplets the outgoing ions can interact with the surrounding He atoms and eventually form stable ionic complexes He + k [22,23].…”

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confidence: 99%

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Interatomic Coulombic decay in helium nanodroplets

et al. 2017

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Interatomic Coulombic decay (ICD) is induced in helium (He) nanodroplets by photoexciting the n = 2 excited state of He + using XUV synchrotron radiation. By recording multiple coincidence electron and ion images we find that ICD occurs in various locations at the droplet surface, inside the surface region, or in the droplet interior. ICD at the surface gives rise to energetic He + ions as previously observed for free He dimers. ICD deeper inside leads to the ejection of slow He + ions due to Coulomb explosion delayed by elastic collisions with neighboring He atoms, and to the formation of He + k complexes.Isolated atoms or molecules excited by energetic radiation typically decay through intramolecular processes such as the emission of an electron or photon. In contrast, in weakly bound complexes, locally generated electrons can additionally interact with neighboring atoms or molecules, leading to new interatomic or intermolecular interactions. Interatomic Coulombic decay (ICD) is a particularly interesting decay process which occurs when local electronic decay is energetically forbidden [1]. Thus, ICD offers a new, ultrafast decay path where energy is exchanged with a neighboring atom leading to its ionization. Since its discovery, ICD has been observed in a wide variety of weakly-bound systems from He dimers [2,3] and rare-gas clusters to biologically relevant systems such as water clusters; for reviews see [4,5]. Today, the focus is on condensed-phase systems where ICD is involved in complex relaxation mechanisms [6][7][8], which can generate genotoxic low-energy electrons and radical cations [9]. Recently, it was suggested to utilize this property of ICD for cancer treatment [10,11].Here we present the first study of ICD in helium (He) nanodroplets. He nanodroplets are generally considered as an ultracold, inert spectroscopic matrix for embedded, isolated molecules and clusters [12,13]. Upon ionization by intense or energetic radiation, however, He droplets turn into a highly reactive medium, inducing reactions and secondary ionization processes of the embedded species [14]. Their homogeneous quantum liquid density profile, and the simple structure of atomic constituents, make He droplets particularly beneficial as benchmark systems for elucidating correlated decay processes. Recent examples include the collective autoionization of multiply excited pure He droplets [15,16] and the creation of doubly charged species by one-photon ionization of doped He droplets [17]. In this work we fully characterize the product states generated by ICD and secondary processes in He nanodroplets using coincidence imaging techniques.The experiments were performed using a He droplet machine attached to a velocity map imaging photoelectron-photoion coincidence (VMI-PEPICO) detector at the GasPhase beamline of Elettra-Sincrotrone Trieste, Italy. The apparatus has been described in detail elsewhere [18,19]. Briefly, a beam of He nanodroplets is produced by continuously expanding pressurized He (50 bar) of high purity He out of a c...

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“…its nearest neighbor due to the steep dependence of the ICD rate on interatomic distance [3]. Three-body effects and more complex interactions give only small contributions [21]. However, in He droplets the outgoing ions can interact with the surrounding He atoms and eventually form stable ionic complexes He + k [22,23].…”

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confidence: 99%

Interatomic Coulombic decay in helium nanodroplets

et al. 2017

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“… 98 , 99 In larger clusters, the computational effort of a full Fano-ADC calculation can further be strongly reduced by combining the Fano-ADC method with the diatomics-in-molecules technique without seriously impairing the accuracy. 116 The application of Stieltjes imaging can generally be avoided by employing the so-called R-matrix method, which uses properly normalized continuum orbitals in constructing scattering wave functions. 117 Alternatively, discrete pseudocontinuum wave functions can be used without renormalization to describe electronic decay in multiply ionized clusters in which the emission of ICD electrons is frustrated by the cluster charge.…”

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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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“…The ICD process and the subsequent Coulomb explosion were simulated with a semiclassical approach combined with a diatomics-in-molecules (DIM) technique. Both are described in detail in [34] and [35], respectively. In brief, the motions of the nuclear quantum wave packets are replaced by a swarm of classical trajectories.…”

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“…The initial conditions are obtained according to the He m ground state nuclear wave functions by Rick et al [37], and the starting potential energy surface is drawn uniformly among all the He + * m electronic excited states. The energy gradients and the ICD rates needed for the propagation are obtained from the DIM technique [35]. The diatomic energies and the ICD rates of He + * 2 (2p) states were taken from [38].…”

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Frustrated Coulomb explosion of small helium clusters

et al. 2018

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Almost ten years ago, energetic neutral hydrogen atoms were detected after a strong-field double ionization of H2. This process, called 'frustrated tunneling ionization', occurs when an ionized electron is recaptured after being driven back to its parent ion by the electric field of a femtosecond laser. In the present study we demonstrate that a related process naturally occurs in clusters without the need of an external field: we observe a charge hopping that occurs during a Coulomb explosion of a small helium cluster, which leads to an energetic neutral helium atom. This claim is supported by theoretical evidence. As an analog to 'frustrated tunneling ionization', we term this process 'frustrated Coulomb explosion'.

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Interatomic Coulombic decay widths of helium trimer: A diatomics-in-molecules approach

Cited by 4 publications

References 59 publications

Interatomic Coulombic decay in helium nanodroplets

Interatomic Coulombic decay in helium nanodroplets

Interatomic and Intermolecular Coulombic Decay

Frustrated Coulomb explosion of small helium clusters

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