Mrug, Eduard (2026) Modeling coarse grained time-resolved fluorescence-detected 2D electronic spectroscopy (F-2DES). Bachelor's Thesis, Physics.
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Abstract
Fluorescence-detected 2D Electronic spectroscopy (F-2DES) is used to study energy transfer in molecular systems, enabling background-free detection with a potential for single-molecule resolution. It results in 2D spectra showing correlations between two laser pulse excitation frequencies. Such spectra for a range of waiting times t2 describe the system dynamics. However, the most important features of the F-2DES spectra, the cross-peaks, are obscured by the dominant Exciton-Exciton Annihilation (EEA) signal. Here, we simulated a well studied LH2 system and found that decreasing the detection time t4 improves the contrast in the 2D spectral evolution. However this effect was only significant once t4 approached EEA timescales, here 0.1 ps. Besides experimental limitations on detection window length, this was at the cost of absolute signal strength, forcing tradeoffs in experimental settings. We also devised a novel experiment, where t2 is fixed (here at 0 fs) and a t4-dependent signal is measured. Simulating such experiment retrieved the inherent fluorescent timescale τF = 986 ps, while normalizing the spectra by one of the peak intensities produced plots containing EEA and exciton dynamics information. The simulated annihilation and transfer parameters were varied to find their influence on these plots. This lays the groundwork for future parameter explorations and more complex fitting in pursuit of recovering the dynamics from an F-2DES experiment without prior knowledge.
| Item Type: | Thesis (Bachelor's Thesis) |
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| Supervisor name: | Jansen, T.L.C. and Gonzalez Migoni, S.C. |
| Degree programme: | Physics |
| Thesis type: | Bachelor's Thesis |
| Language: | English |
| Date Deposited: | 05 Aug 2026 06:34 |
| Last Modified: | 05 Aug 2026 06:34 |
| URI: | https://fse.studenttheses.ub.rug.nl/id/eprint/37479 |
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