Internal energy dependence in x-ray-induced molecular fragmentation: An experimental and theoretical study of thiophene

E. Kukk, D. T. Ha, Y. Wang, D. G. Piekarski, S. Diaz-Tendero, K. Kooser, E. Itälä, H. Levola, M. Alcamí, E. Rachlew, and F. Martín
Phys. Rev. A 91, 043417 – Published 24 April 2015
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Abstract

A detailed experimental and theoretical investigation of the dynamics leading to fragmentation of doubly ionized molecular thiophene is presented. Dissociation of double-ionized molecules was induced by S 2p core photoionization and the ionic fragments were detected in coincidence with Auger electrons from the core-hole decay. Rich molecular dynamics was observed in electron-ion-ion coincidence maps exhibiting ring breaks accompanied by hydrogen losses and/or migration. The probabilities of various dissociation channels were seen to be very sensitive to the internal energy of the molecule. Theoretical simulations were performed by using the semiempirical self-consistent charge-density-functional tight-binding method. By running thousands of these simulations, the initial conditions encountered in the experiment were properly taken into account, including the systematic dependencies on the internal (thermal) energy. This systematic approach, not affordable with first-principle methods, provides a good overall description of the complex molecular dynamics observed in the experiment and shows good promise for applicability to larger molecules or clusters, thus opening the door to systematic investigations of complex dynamical processes occurring in radiation damage.

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  • Received 10 February 2015

DOI:https://doi.org/10.1103/PhysRevA.91.043417

©2015 American Physical Society

Authors & Affiliations

E. Kukk1,*, D. T. Ha2, Y. Wang2,3, D. G. Piekarski2, S. Diaz-Tendero2, K. Kooser1, E. Itälä1, H. Levola1, M. Alcamí2, E. Rachlew4, and F. Martín2,3,5

  • 1Department of Physics and Astronomy, University of Turku, FIN-20014 Turku, Finland
  • 2Departamento de Química, Módulo 13, Universidad Autónoma de Madrid, Cantoblanco 28049 Madrid, Spain
  • 3Instituto Madrileño de Estudios Avanzados en Nanociencia, Cantoblanco, 28049 Madrid, Spain
  • 4Atomic and Molecular Physics, Royal Institute of Technology KTH, Stockholm, Sweden
  • 5Condensed Matter Physics Center (IFIMAC), Universidad Autónoma de Madrid, 28049 Madrid, Spain

  • *edwin.kukk@utu.fi; Turku University Centre for Materials and Surfaces (MATSURF).

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Issue

Vol. 91, Iss. 4 — April 2015

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