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Title: Electron–vibration coupling induced renormalization in the photoemission spectrum of diamondoids

The development of theories and methods devoted to the accurate calculation of the electronic quasi-particle states and levels of molecules, clusters and solids is of prime importance to interpret the experimental data. These quantum systems are often modelled by using the Born–Oppenheimer approximation where the coupling between the electrons and vibrational modes is not fully taken into account, and the electrons are treated as pure quasi-particles. Here, we show that in small diamond cages, called diamondoids, the electron–vibration coupling leads to the breakdown of the electron quasi-particle picture. More importantly, we demonstrate that the strong electron–vibration coupling is essential to properly describe the overall lineshape of the experimental photoemission spectrum. This cannot be obtained by methods within Born–Oppenheimer approximation. Furthermore, we deduce a link between the vibronic states found by our many-body perturbation theory approach and the well-known Jahn–Teller effect.
Authors:
ORCiD logo [1] ;  [2] ;  [3] ;  [1] ;  [4] ;  [5]
  1. Hungarian Academy of Sciences, Budapest (Hungary); Univ. of Technology and Economics, Budapest (Hungary)
  2. Hungarian Academy of Sciences, Budapest (Hungary); Lorand Eotvos Univ., Budapest (Hungary)
  3. Argonne National Lab. (ANL), Lemont, IL (United States); Univ. of Chicago, Chicago, IL (United States)
  4. Aix-Marseille Univ., Marseille (France)
  5. Institute for Material Science (ISM) of the National Research Council (CNR), Monterotondo Stazione (Italy)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1352526