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Signatures of Exciton Delocalization and Exciton-Exciton Annihilation in Fluorescence-Detected Two-Dimensional Coherent Spectroscopy.
| Content Provider | Semantic Scholar |
|---|---|
| Author | Malý, Pavel Mančal, Tomáš |
| Copyright Year | 2018 |
| Abstract | Incoherently detected coherent multidimensional spectroscopy is rapidly gaining popularity, promising a different application range and sensitivity than its traditional counterpart. While measuring the same response, the two methods are not equivalent. 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 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. Strictly on the basis of time-dependent perturbation theory, we study how in both methods the varying degree of cancellation between perturbative contributions gives rise to cross-peaks and we 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 the annihilation contribution itself. |
| Starting Page | 5654 |
| Ending Page | 5659 |
| Page Count | 6 |
| File Format | PDF HTM / HTML |
| PubMed reference number | 30188728 |
| Journal | Medline |
| Volume Number | 9 |
| Issue Number | 19 |
| Alternate Webpage(s) | https://arxiv.org/pdf/1807.04846v1.pdf |
| Alternate Webpage(s) | https://export.arxiv.org/pdf/1807.04846 |
| Alternate Webpage(s) | https://doi.org/10.1021/acs.jpclett.8b02271 |
| Journal | The journal of physical chemistry letters |
| Language | English |
| Access Restriction | Open |
| Content Type | Text |
| Resource Type | Article |
