Signatures of Exciton Delocalization and Exciton-Exciton Annihilation in Fluorescence-Detected Two-Dimensional Coherent Spectroscopy
| Autor: | Mal��, Pavel, Man��al, Tom���� |
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| Rok vydání: | 2018 |
| Předmět: | |
| DOI: | 10.48550/arxiv.1807.04846 |
| Popis: | We present calculations of the fluorescence-detected coherent two-dimensional (F-2DES) spectra of a molecular heterodimer. We compare how the F-2DES technique differs from the standard coherently detected two-dimensional (2DES) spectroscopy in measuring exciton delocalization. We analyze which processes contribute to cross-peaks in the zero-waiting-time spectra obtained by the two methods. Based strictly on time-dependent perturbation theory, we study how in both methods varying degree of cancellation between perturbative contributions gives rise to cross-peaks, and identify exciton annihilation and exciton relaxation contributions to the cross-peak in the zero-waiting-time F-2DES. We propose that time-gated fluorescence detection can be used to isolate the annihilation contribution to F-2DES both to retrieve information equivalent to 2DES spectroscopy and to study annihilation contribution itself. 12 pages including SI, 4 figures and 1 table |
| Databáze: | OpenAIRE |
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