Two-dimensional Fano lineshapes : Excited-state absorption contributions
(2018) In Journal of Chemical Physics 148(18).- 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... (More)
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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- author
- Finkelstein-Shapiro, Daniel LU ; Pullerits, Tõnu LU and Hansen, Thorsten LU
- organization
- publishing date
- 2018-05-14
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Journal of Chemical Physics
- volume
- 148
- issue
- 18
- article number
- 184201
- publisher
- American Institute of Physics (AIP)
- external identifiers
-
- pmid:29764148
- scopus:85046889490
- ISSN
- 0021-9606
- DOI
- 10.1063/1.5019376
- language
- English
- LU publication?
- yes
- id
- 0ad5c1cf-fdad-4d0b-be75-1091a0ed1c7b
- date added to LUP
- 2018-05-23 13:37:46
- date last changed
- 2024-09-02 20:45:01
@article{0ad5c1cf-fdad-4d0b-be75-1091a0ed1c7b,
abstract = {{<p>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.</p>}},
author = {{Finkelstein-Shapiro, Daniel and Pullerits, Tõnu and Hansen, Thorsten}},
issn = {{0021-9606}},
language = {{eng}},
month = {{05}},
number = {{18}},
publisher = {{American Institute of Physics (AIP)}},
series = {{Journal of Chemical Physics}},
title = {{Two-dimensional Fano lineshapes : Excited-state absorption contributions}},
url = {{http://dx.doi.org/10.1063/1.5019376}},
doi = {{10.1063/1.5019376}},
volume = {{148}},
year = {{2018}},
}