Interatomic electronic decay processes in singly and multiply ionized clusters

Averbukh, Vitali; Demekhin, Ph. V.; Kolorenč, Přemysl; Scheit, S.; Stoychev, Spas D.; Kuleff, Alexander I.; Chiang, Ying‐Chih; Gokhberg, Kirill; Kopelke, S.; Sisourat, Nicolas; Cederbaum, Lorenz S.

doi:10.1016/j.elspec.2010.03.003

Cited by 90 publications

(82 citation statements)

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“…The discovery of the ICD revealed a whole zoo of related phenomena, involving both energy and electron transfer and initiated by single or multiple ionization, as well as by inner-or outer valence excitation (for recent review, see Ref. [6]). Although these processes have different names and acronyms, we will refer here to all these phenomena as ICD in order to make the text more transparent.…”

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Ultrafast Interatomic Electronic Decay in Multiply Excited Clusters

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An ultrafast mechanism belonging to the family of interatomic Coulombic decay (ICD) phenomena is proposed. When two excited species are present, an ultrafast energy transfer can take place bringing one of them to its ground state and ionizing the other one. It is shown that if large homoatomic clusters are exposed to an ultrashort and intense laser pulse whose photon energy is in resonance with an excitation transition of the cluster constituents, the large majority of ions will be produced by this ICD mechanism rather than by two-photon ionization. A related collective-ICD process that is operative in heteroatomic systems is also discussed.PACS numbers: 31.70. Hq, 32.80.Rm, 32.80.Wr The rapid development during the last decades of very intense light sources with extreme short pulse duration opened a new era in the study of radiation-matter interaction. Studying the interaction of intense fields with matter brought to the discovery of a whole plethora of new physical phenomena, like high-harmonic generation, above-threshold ionization, or tunneling ionization, to name only a few. In the same time, the progress in generating extremely short pulses gave the scientific community a powerful tool to monitor and control the electron dynamics in atomic and molecular systems and to study processes that take place on a time scale in which the electronic motion is still disentangled from the slower nuclear dynamics (for recent reviews see, e.g., Refs. [1, 2]). A number of free-electron lasers are in operation today providing extremely bright, coherent, and ultrashort pulses in the VUV regime. Exposed to such highly intense pulses, atomic and molecular systems will absorb a large amount of photons triggering various dynamical effects. In this letter we will restrict ourselves to situations where the single-photon energy in the pulse is not high enough to directly ionize the system. It is well known that even in this case the system can be ionized by a multiphoton ionization mechanism. The multiphoton ionization (MPI) results from the ability of quantum systems to absorb several and even many photons, whose individual energies are insufficient to ionize the system. The combined energy of the absorbed photons, though, suffices to eventually eject one or many electrons from the system. During the last decade the MPI has been intensively studied also in composite systems, like clusters, employing the new powerful laser sources (for a review see, e.g. Ref.[3]). However, little attention was paid to other mechanisms that can lead to a multiple ionization in an atomic or molecular cluster irradiated by an intense laser pulse.In this letter we aim at discussing a hitherto unrecognized mechanism for producing ionized species in homoatomic or homomolecular clusters exposed to an intense laser pulse, which in many cases can be by far One of the constituents of the system de-excites transferring the energy to the neighbor which uses it to emit its excited electron.the dominating one. For simplicity we will consider an atomic cluste...

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“…Refs. [5][6][7][8][9][10]). The ICD is a very efficient electronic decay mode of inner-valence ionized atoms or molecules embedded in an environment.…”

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Ultrafast Interatomic Electronic Decay in Multiply Excited Clusters

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“…An experimentalist point of view review of the "early years of ICD" can be found in [10] and of more recent studies in [11]. Two comprehensive theoretical review papers by Santra et al [12] and Averbukh et al [13] are available, as well.…”

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A comprehensive study of Interatomic Coulombic Decay in argon dimers: Extracting R-dependent absolute decay rates from the experiment

et al. 2017

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In this work we present a comprehensive and detailed study of Interatomic Coulombic Decay (ICD) occurring after irradiating argon dimers with XUV-synchrotron radiation. A manifold of different decay channels is observed and the corresponding initial and final states are assigned.Additionally, the effect of nuclear dynamics on the ICD electron spectrum is examined for one specific decay channel. The internuclear distance-dependent width Γ(R) of the decay is obtained from the measured energy distribution employing a classical nuclear dynamics model.

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“…For the final states in question, the relevant limit is the sum of the binding energies of both outer valence electrons taking part in the decay, to which the Coulomb repulsion energy of the two vacancies in the final state needs to be added. 2,7,8,11,12 Therefore, the total energy of the final state in the case of ICD can be lower than in Auger decay, because the Coulomb energy of the distributed vacancies in the ICD case is lower than the one of a localized two-hole state in the Auger case. Singly ionized 3 states which cannot decay by Auger emission can be unstable against ICD.…”

Section: Introductionmentioning

confidence: 99%

“…In the last decade it has been found that new autoionization channels can indeed open up in such a case, leading to final states with one vacancy located at the site of original ionization and the other on a neighboring atom or molecule. [2][3][4][5][6][7][8] Typically, such a transition occurs at lower energy than most Auger processes and starts out from the ionization of an inner valence level. Both final state vacancies are located in outer valence levels.…”

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confidence: 99%

Interatomic Coulombic decay in mixed NeKr clusters

Arion

Mucke

Förstel

et al. 2011

The Journal of Chemical Physics

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We report the occurrence of Interatomic Coulombic Decay (ICD) in mixed NeKr clusters. A well-defined feature ranging from 9 -12 eV in kinetic energy is observed in coincidence with the Ne 2s photoelectrons. It derives from an ICD process, in which an initial Ne 2s vacancy is filled by a Ne 2p electron and an electron is emitted from a 4p level on a neighboring Kr atom. We have studied the dependence of the effect on photon energy, cluster composition and cluster size. Interestingly, the ICD electron energy increases slightly and grows a shoulder on going from 2% to 5% Kr in the co-expansion process, which we interpret in terms of surface vs. bulk effects.

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Interatomic electronic decay processes in singly and multiply ionized clusters

Cited by 90 publications

References 75 publications

Ultrafast Interatomic Electronic Decay in Multiply Excited Clusters

Ultrafast Interatomic Electronic Decay in Multiply Excited Clusters

A comprehensive study of Interatomic Coulombic Decay in argon dimers: Extracting R-dependent absolute decay rates from the experiment

Interatomic Coulombic decay in mixed NeKr clusters

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