%0 Journal Article %1 suss2020excitonexciton %A Süß, J %A Engel, V %B The Journal of Chemical Physics %D 2020 %I American Institute of Physics %J J. Chem. Phys. %K ak-engel grk1221 myown %N 16 %P 164310 %R 10.1063/5.0027837 %T Exciton–exciton annihilation in a molecular trimer: Wave packet dynamics and 2D spectroscopy %U https://doi.org/10.1063/5.0027837 %V 153 %X We theoretically study the exciton–exciton annihilation (EEA) in a molecular trimer MMM. The system is treated within a model of electronic states, and the coupling to a bath is incorporated using the quantum jump method. Two situations of initial excitation are compared. In the first one, a two-photon process populates configurations M*M*M and MM*M* so that two excitons reside on neighboring monomers M. Then, EEA can immediately proceed. In contrast, if the trimer initially is in the local configuration M*MM*, exciton diffusion must occur before the annihilation process can take place. For the trimer, this excitonic motion takes place on a very short time scale. In both cases, wave packets are prepared which show a different quantum dynamics where the latter depends on the couplings and decay rates. It is documented how fifth-order coherent two-dimensional spectroscopy can be used to directly map the EEA as a function of time.

@article{suss2020excitonexciton, abstract = {We theoretically study the exciton–exciton annihilation (EEA) in a molecular trimer MMM. The system is treated within a model of electronic states, and the coupling to a bath is incorporated using the quantum jump method. Two situations of initial excitation are compared. In the first one, a two-photon process populates configurations M*M*M and MM*M* so that two excitons reside on neighboring monomers M. Then, EEA can immediately proceed. In contrast, if the trimer initially is in the local configuration M*MM*, exciton diffusion must occur before the annihilation process can take place. For the trimer, this excitonic motion takes place on a very short time scale. In both cases, wave packets are prepared which show a different quantum dynamics where the latter depends on the couplings and decay rates. It is documented how fifth-order coherent two-dimensional spectroscopy can be used to directly map the EEA as a function of time.}, added-at = {2020-11-02T17:27:30.000+0100}, author = {Süß, J and Engel, V}, biburl = {https://www.bibsonomy.org/bibtex/2d4a16b1ee324db01111a12992794faeb/ak-engel-uniwue}, booktitle = {The Journal of Chemical Physics}, comment = {doi: 10.1063/5.0027837}, doi = {10.1063/5.0027837}, interhash = {3c6c34acb78501fb365393db4ec60b3b}, intrahash = {d4a16b1ee324db01111a12992794faeb}, issn = {00219606}, journal = {J. Chem. Phys.}, keywords = {ak-engel grk1221 myown}, month = oct, number = 16, pages = 164310, publisher = {American Institute of Physics}, timestamp = {2021-07-19T18:50:41.000+0200}, title = {Exciton–exciton annihilation in a molecular trimer: Wave packet dynamics and 2D spectroscopy}, url = {https://doi.org/10.1063/5.0027837}, volume = 153, year = 2020 }