Two-dimensional Fano lineshapes: Excited-state absorption contributions

The Journal of Chemical Physics
Daniel Finkelstein-ShapiroThorsten Hansen

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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Citations

Aug 11, 2020·The Journal of Chemical Physics·Lev Chuntonov, Igor V Rubtsov
Jul 26, 2018·The Journal of Physical Chemistry Letters·Bar CohnLev Chuntonov
Jul 14, 2020·The Journal of Physical Chemistry Letters·Gökçen Tek, Peter Hamm

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