Ultralong-range energy transfer by interatomic Coulombic decay in an extreme quantum system

Sisourat, Nicolas; Kryzhevoi, Nikolai V.; Kolorenč, Přemysl; Scheit, S.; Jahnke, T.; Cederbaum, Lorenz S.

doi:10.1038/nphys1685

Cited by 148 publications

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“…Ion-ion-electron coincidence time-of-flight mass spectrum recorded at hν = 67.5 eV and for a mean droplet size of N = 4000 He atoms. The inset shows photoelectron spectra measured in coincidence with He + for various N and for free He2 [3]. its nearest neighbor due to the steep dependence of the ICD rate on interatomic distance [3].…”

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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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“…The inset shows photoelectron spectra measured in coincidence with He + for various N and for free He2 [3]. 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].…”

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Interatomic Coulombic decay in helium nanodroplets

et al. 2017

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“…Another striking feature of this process is that ICD remains effective for considerable interatomic distances. ICD was demonstrated experimentally and theoretically for He dimer, which is the weakest bound system known in nature, and found to be operative over distances of about 45 times the atomic radius [4,5].…”

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Site- and energy-selective slow-electron production through intermolecular Coulombic decay

Gokhberg

Kolorenč

Kuleff

et al. 2013

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Since its discovery in 1997 [1], the ICD has been successfully investigated in a variety of systems [2]. It usually proceeds on a femtosecond timescale and becomes faster the more neighbors are present, dominating most of the competing relaxation processes. Experimental investigation of ICD in water dimers [3] found the rate of this process to be so large as to completely suppress the proton transfer in the inner-valence ionized water molecules.As a result of ICD, two intact water cations are produced by the consecutive Coulomb 1

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“…Prominent examples can be found in [38][39][40]). For NeAr dimers Ouchi et al [41] used even the relative height of two peaks in the KER distribution to test calculated decay width very directly.…”

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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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Ultralong-range energy transfer by interatomic Coulombic decay in an extreme quantum system

Cited by 148 publications

References 20 publications

Interatomic Coulombic decay in helium nanodroplets

Interatomic Coulombic decay in helium nanodroplets

Site- and energy-selective slow-electron production through intermolecular Coulombic decay

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

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