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Simulating Fluorescence-Detected Two-Dimensional Electronic Spectroscopy of Multichromophoric Systems
Tenzin Kunsel1, Vivek Tiwari2, Yassel Acosta Matutes2
1Zernike Institute for Advanced Materials , University of Groningen , Nijenborgh 4 , 9747 AG Groningen , The Netherlands.
The Journal of Physical Chemistry. B
|December 14, 2018
Summary
We developed a theory for modeling fluorescence-detected 2D electronic spectroscopy in light-harvesting complexes. This approach explains strong cross-peaks by exciton annihilation, enabling new studies of energy transfer dynamics.
Area of Science:
- Quantum Biology and Spectroscopy
- Photophysics of Light-Harvesting Systems
Background:
- Understanding energy transfer in multichromophoric systems is crucial for photosynthesis and artificial light-harvesting.
- Conventional 2D electronic spectroscopy (2DES) provides insights but can be obscured by complex signal contributions.
Purpose of the Study:
- To develop and validate a theoretical framework for fluorescence-detected 2D electronic spectroscopy (FD-2DES) in multichromophoric systems.
- To elucidate the origin of strong cross-peaks observed in FD-2DES spectra of the light-harvesting complex LH2.
Main Methods:
- Development of a theoretical model for FD-2DES.
- Comparison of theoretical predictions with experimental data for the LH2 complex.
- Analysis of exciton dynamics, including annihilation and relaxation processes.
Main Results:
- The theory successfully models FD-2DES spectra of LH2, accurately reproducing experimental data.
- Strong cross-peaks in FD-2DES are attributed to exciton-exciton annihilation, which cleans the ground-state signal.
- Line shape differences are explained by slow dynamics, exciton delocalization, and intraband exciton-exciton annihilation.
Conclusions:
- FD-2DES offers a powerful method to study exciton dynamics in light-harvesting complexes.
- Exciton-exciton annihilation plays a significant role in shaping the observed spectral features.
- Time-resolved FD-2DES is proposed as a tool for state-resolved exciton-exciton annihilation studies.
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