Signatures of Exciton Delocalization and Exciton-Exciton Annihilation in Fluorescence-Detected Two-Dimensional Coherent Spectroscopy

Result code in IS VaVaI
<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F18%3A10389009" target="_blank" >RIV/00216208:11320/18:10389009 - isvavai.cz</a>
Result on the web
<a href="https://doi.org/10.1021/acs.jpclett.8b02271" target="_blank" >https://doi.org/10.1021/acs.jpclett.8b02271</a>
DOI - Digital Object Identifier
<a href="http://dx.doi.org/10.1021/acs.jpclett.8b02271" target="_blank" >10.1021/acs.jpclett.8b02271</a>

Result language
angličtina
Original language name
Signatures of Exciton Delocalization and Exciton-Exciton Annihilation in Fluorescence-Detected Two-Dimensional Coherent Spectroscopy
Original language description
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.
Czech name
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Czech description
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Type
J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database
CEP classification
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OECD FORD branch
10301 - Atomic, molecular and chemical physics (physics of atoms and molecules including collision, interaction with radiation, magnetic resonances, Mössbauer effect)

Project
<a href="/en/project/GA17-22160S" target="_blank" >GA17-22160S: Quantum theory of excitation energy transfer and advanced optical spectroscopy: from small dye molecules to light-harvesting complexes</a><br>
Continuities
P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Publication year
2018
Confidentiality
S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

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