Two-dimensional Fano lineshapes : Excited-state absorption contributions

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.

• Author: Daniel Finkelstein-Shapiro; Tõnu Pullerits; Thorsten Hansen
• 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
• Links: http://dx.doi.org/10.1063/1.5019376
• Document type: Journal article
• Publisher: American Institute of Physics (AIP)
• Topic: Physical Chemistry (including Surface- and Colloid Chemistry); Atom and Molecular Physics and Optics
• Status: Published
• ISBN/ISSN/Other: ISSN: 0021-9606