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Portrait of Tönu Pullerits; Photo: Kennet Ruona

Tönu Pullerits

Professor

Portrait of Tönu Pullerits; Photo: Kennet Ruona

Two-dimensional Fano lineshapes : Excited-state absorption contributions

Author

  • Daniel Finkelstein-Shapiro
  • Tõnu Pullerits
  • Thorsten Hansen

Summary, in English

Fano interferences in nanostructures are influenced by dissipation effects as well as many-body interactions. Two-dimensional coherent spectroscopies have just begun to be applied to these systems where the spectroscopic signatures of a discrete-continuum structure are not known. In this article, we calculate the excited-state absorption contribution for different models of higher lying excited states. We find that the characteristic asymmetry of one-dimensional spectroscopies is recovered from the many-body contributions and that the higher lying excited manifolds have distorted lineshapes that are not anticipated from discrete-level Hamiltonians. We show that the Stimulated Emission cannot have contributions from a flat continuum of states. This work completes the Ground-State Bleach and Stimulated Emission signals that were calculated previously [D. Finkelstein-Shapiro et al., Phys. Rev. B 94, 205137 (2016)]. The model reproduces the observations reported for molecules on surfaces probed by 2DIR.

Department/s

  • Chemical Physics
  • eSSENCE: The e-Science Collaboration

Publishing year

2018-05-14

Language

English

Publication/Series

Journal of Chemical Physics

Volume

148

Issue

18

Document type

Journal article

Publisher

American Institute of Physics (AIP)

Topic

  • Physical Chemistry
  • Atom and Molecular Physics and Optics

Status

Published

ISBN/ISSN/Other

  • ISSN: 0021-9606