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Two-dimensional Fano lineshapes: Excited-state absorption contributions.

Authors :
Finkelstein-Shapiro, Daniel
Pullerits, Tõnu
Hansen, Thorsten
Source :
Journal of Chemical Physics; 5/14/2018, Vol. 148 Issue 18, pN.PAG-N.PAG, 10p, 4 Diagrams, 2 Charts, 4 Graphs
Publication Year :
2018

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 <italic>et al.</italic>, Phys. Rev. B <bold>94</bold>, 205137 (2016)]. The model reproduces the observations reported for molecules on surfaces probed by 2DIR. [ABSTRACT FROM AUTHOR]

Details

Language :
English
ISSN :
00219606
Volume :
148
Issue :
18
Database :
Complementary Index
Journal :
Journal of Chemical Physics
Publication Type :
Academic Journal
Accession number :
129603518
Full Text :
https://doi.org/10.1063/1.5019376