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Published on: May 7, 2017
Two-dimensional Fano lineshapes: Excited-state absorption contributions.
Daniel Finkelstein-Shapiro1, Tõnu Pullerits1, Thorsten Hansen2
1Division of Chemical Physics, Lund University, P.O. Box 124, 221 00 Lund, Sweden.
This study explores Fano interferences in nanostructures using advanced spectroscopy. We reveal how many-body interactions and higher excited states distort spectral lineshapes, clarifying complex spectroscopic signatures.
Area of Science:
- Quantum optics
- Condensed matter physics
- Spectroscopy
Background:
- Fano interferences in nanostructures are complex, influenced by dissipation and many-body interactions.
- Two-dimensional coherent spectroscopy (2DIR) is emerging for studying these systems, but their spectral signatures are not well understood.
Purpose of the Study:
- To calculate the excited-state absorption contribution in nanostructure Fano interferences.
- To elucidate the role of many-body interactions and higher excited states on spectroscopic signatures.
- To complete previous calculations of Ground-State Bleach and Stimulated Emission signals.
Main Methods:
- Theoretical calculation of excited-state absorption contributions.
- Modeling of higher lying excited states in nanostructure systems.
- Analysis of many-body contributions to spectroscopic features.
Main Results:
- The characteristic asymmetry of 1D spectroscopies is recovered due to many-body contributions.
- Higher excited manifolds exhibit distorted lineshapes not predicted by simple discrete-level models.
- Stimulated Emission signals do not arise from flat continuum states.
Conclusions:
- The developed model accurately reproduces experimental observations of molecules on surfaces probed by 2DIR.
- This work provides a theoretical framework for interpreting complex 2DIR spectra of nanostructures.
- Understanding these many-body effects is crucial for characterizing quantum phenomena in nanostructures.
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