Two-dimensional Fano lineshapes: Excited-state absorption contributions

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Abstract

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.

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  • University of Copenhagen
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Subject classification (UKÄ) – MANDATORY

  • Physical Chemistry
Original languageEnglish
Article number184201
JournalJournal of Chemical Physics
Volume148
Issue number18
Publication statusPublished - 2018 May 14
Publication categoryResearch
Peer-reviewedYes