%0 Journal Article %1 dostal2018direct %A Dostál, Jakub %A Fennel, Franziska %A Koch, Federico %A Herbst, Stefanie %A Würthner, Frank %A Brixner, Tobias %D 2018 %J Nature Communications %K cells molecular myown photovoltaic %N 1 %P 2466--2473 %R 10.1038/s41467-018-04884-4 %T Direct observation of exciton–exciton interactions %U https://doi.org/10.1038/s41467-018-04884-4 %V 9 %X Natural light harvesting as well as optoelectronic and photovoltaic devices depend on efficient transport of energy following photoexcitation. Using common spectroscopic methods, however, it is challenging to discriminate one-exciton dynamics from multi-exciton interactions that arise when more than one excitation is present in the system. Here we introduce a coherent two-dimensional spectroscopic method that provides a signal only in case that the presence of one exciton influences the behavior of another one. Exemplarily, we monitor exciton diffusion by annihilation in a perylene bisimide-based J-aggregate. We determine quantitatively the exciton diffusion constant from exciton–exciton-interaction 2D spectra and reconstruct the annihilation-free dynamics for large pump powers. The latter enables for ultrafast spectroscopy at much higher intensities than conventionally possible and thus improves signal-to-noise ratios for multichromophore systems; the former recovers spatio–temporal dynamics for a broad range of phenomena in which exciton interactions are present.

@article{dostal2018direct, abstract = {Natural light harvesting as well as optoelectronic and photovoltaic devices depend on efficient transport of energy following photoexcitation. Using common spectroscopic methods, however, it is challenging to discriminate one-exciton dynamics from multi-exciton interactions that arise when more than one excitation is present in the system. Here we introduce a coherent two-dimensional spectroscopic method that provides a signal only in case that the presence of one exciton influences the behavior of another one. Exemplarily, we monitor exciton diffusion by annihilation in a perylene bisimide-based J-aggregate. We determine quantitatively the exciton diffusion constant from exciton–exciton-interaction 2D spectra and reconstruct the annihilation-free dynamics for large pump powers. The latter enables for ultrafast spectroscopy at much higher intensities than conventionally possible and thus improves signal-to-noise ratios for multichromophore systems; the former recovers spatio–temporal dynamics for a broad range of phenomena in which exciton interactions are present.}, added-at = {2018-06-28T11:47:19.000+0200}, author = {Dostál, Jakub and Fennel, Franziska and Koch, Federico and Herbst, Stefanie and Würthner, Frank and Brixner, Tobias}, biburl = {https://www.bibsonomy.org/bibtex/2d65c831e7630149c262ed741b97f9b30/wuerthner_group}, doi = {10.1038/s41467-018-04884-4}, interhash = {44671ba92666a2293af5cba2a5e6d351}, intrahash = {d65c831e7630149c262ed741b97f9b30}, issn = {20411723}, journal = {Nature Communications}, keywords = {cells molecular myown photovoltaic}, month = jun, number = 1, pages = {2466--2473}, refid = {Dostál2018}, timestamp = {2018-07-09T11:00:04.000+0200}, title = {Direct observation of exciton–exciton interactions}, url = {https://doi.org/10.1038/s41467-018-04884-4}, volume = 9, year = 2018 }