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

Abstract

In this paper 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 kinetic energy release distribution of the ions employing a classical nuclear dynamics model.

Authors:
 [1];  [2];  [3];  [1];  [1];  [4];  [1];  [5];  [6];  [6];  [1];  [6];  [3];  [3];  [5];  [1];  [7];  [8];  [2];  [1] more »;  [1] « less
  1. Goethe Univ., Frankfurt (Germany)
  2. Heidelberg Univ. (Germany)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Goethe Univ., Frankfurt (Germany); Auburn Univ., AL (United States)
  5. Auburn Univ., AL (United States)
  6. Kansas State Univ., Manhattan, KS (United States)
  7. Reno Univ., NV (United States)
  8. Charles Univ., Prague (Czech Republic). Faculty of Mathematics and Physics
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1379680
Grant/Contract Number:
AC02-05CH11231; FG02-86ER13491
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Chemical Physics
Additional Journal Information:
Journal Volume: 482; Journal Issue: C; Journal ID: ISSN 0301-0104
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Rist, J., Miteva, T., Gaire, B., Sann, H., Trinter, F., Keiling, M., Gehrken, N., Moradmand, A., Berry, B., Zohrabi, M., Kunitski, M., Ben-Itzhak, I., Belkacem, A., Weber, T., Landers, A. L., Schöffler, M., Williams, J. B., Kolorenč, P., Gokhberg, K., Jahnke, T., and Dörner, R. A comprehensive study of Interatomic Coulombic Decay in argon dimers: Extracting R-dependent absolute decay rates from the experiment. United States: N. p., 2016. Web. doi:10.1016/j.chemphys.2016.09.024.
Rist, J., Miteva, T., Gaire, B., Sann, H., Trinter, F., Keiling, M., Gehrken, N., Moradmand, A., Berry, B., Zohrabi, M., Kunitski, M., Ben-Itzhak, I., Belkacem, A., Weber, T., Landers, A. L., Schöffler, M., Williams, J. B., Kolorenč, P., Gokhberg, K., Jahnke, T., & Dörner, R. A comprehensive study of Interatomic Coulombic Decay in argon dimers: Extracting R-dependent absolute decay rates from the experiment. United States. doi:10.1016/j.chemphys.2016.09.024.
Rist, J., Miteva, T., Gaire, B., Sann, H., Trinter, F., Keiling, M., Gehrken, N., Moradmand, A., Berry, B., Zohrabi, M., Kunitski, M., Ben-Itzhak, I., Belkacem, A., Weber, T., Landers, A. L., Schöffler, M., Williams, J. B., Kolorenč, P., Gokhberg, K., Jahnke, T., and Dörner, R. 2016. "A comprehensive study of Interatomic Coulombic Decay in argon dimers: Extracting R-dependent absolute decay rates from the experiment". United States. doi:10.1016/j.chemphys.2016.09.024. https://www.osti.gov/servlets/purl/1379680.
@article{osti_1379680,
title = {A comprehensive study of Interatomic Coulombic Decay in argon dimers: Extracting R-dependent absolute decay rates from the experiment},
author = {Rist, J. and Miteva, T. and Gaire, B. and Sann, H. and Trinter, F. and Keiling, M. and Gehrken, N. and Moradmand, A. and Berry, B. and Zohrabi, M. and Kunitski, M. and Ben-Itzhak, I. and Belkacem, A. and Weber, T. and Landers, A. L. and Schöffler, M. and Williams, J. B. and Kolorenč, P. and Gokhberg, K. and Jahnke, T. and Dörner, R.},
abstractNote = {In this paper 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 kinetic energy release distribution of the ions employing a classical nuclear dynamics model.},
doi = {10.1016/j.chemphys.2016.09.024},
journal = {Chemical Physics},
number = C,
volume = 482,
place = {United States},
year = 2016,
month = 9
}

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  • In the present paper, we show that the absorption of a single photon can singly ionize both atoms of a helium dimer (He{sub 2}): ionization with simultaneous excitation of one atom followed by de-excitation via interatomic Coulombic decay leads to the ejection of an electron from each of the the two atoms of the dimer. Using the Cold Target Recoil Ion Momentum Spectroscopy technique (COLTRIMS), we obtained angular distributions of these electrons in the laboratory frame and the molecular frame. We observe a pronounced variation of these distributions for different regions of kinetic-energy releases of the ions.
  • Interatomic Coulombic decay (ICD) is observed in the rare gas homonuclear dimers Ar{sub 2}, Kr{sub 2}, and Xe{sub 2} with photoion spectroscopy techniques. Inner valence ionization of the outer ns shell of these systems is known to create a metastable state that dissociates to form a ground state ion and a neutral excited fragment. Inner valence ionization to form ns satellite states leads to similar dissociations, but the neutral fragment gets all the more excited as the internal energy of the ns satellite state increases. When enough excitation energy is transferred to reach the ionization potential, ICD occurs. ICD thresholdmore » is observed to coincide with the position of the A{sup +}A{sup +} ground state in the Franck-Condon region.« less
  • A scheme utilizing excitation of core electrons followed by the resonant-Auger – interatomic Coulombic decay (RA-ICD) cascade was recently proposed as a means of controlling the generation site and energies of slow ICD electrons. This control mechanism was verified in a series of experiments in rare gas dimers. In this article, we present fully ab initio computed ICD electron and kinetic energy release spectra produced following 2p{sub 3/2} → 4s, 2p{sub 1/2} → 4s, and 2p{sub 3/2} → 3d core excitations of Ar in Ar{sub 2}. We demonstrate that the manifold of ICD states populated in the resonant Auger processmore » comprises two groups. One consists of lower energy ionization satellites characterized by fast interatomic decay, while the other consists of slow decaying higher energy ionization satellites. We show that accurate description of nuclear dynamics in the latter ICD states is crucial for obtaining theoretical electron and kinetic energy release spectra in good agreement with the experiment.« less
  • Electronically excited atom or molecule in an environment can relax via transferring its excess energy to the neighboring atoms or molecules. The process is called Interatomic or Intermolecular coulombic decay (ICD). The ICD is a fast decay process in environment. Generally, the ICD mechanism predominates in weakly bound clusters. In this paper, we have applied the complex absorbing potential approach/equation-of-motion coupled cluster (CAP/EOMCCSD) method which is a combination of CAP and EOMCC approach to study the lifetime of ICD at various geometries of the molecules. We have applied this method to calculate the lifetime of ICD in Ne-X; X =more » Ne, Mg, Ar, systems. We compare our results with other theoretical and experimental results available in literature.« less