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- W2056146543 abstract "The interaction of exciton and charge transfer (CT) states plays a central role in photo-induced CT processes in chemistry, biology and physics. In this work, we use a combination of two-dimensional electronic spectroscopy (2D-ES), pump-probe measurements and quantum chemistry to investigate the ultrafast CT dynamics in a lutetium bisphthalocyanine dimer in different oxidation states. It is found that in the anionic form, the combination of strong CT-exciton interaction and electronic asymmetry induced by a counter-ion enables CT between the two macrocycles of the complex on a 30 fs timescale. Following optical excitation, a chain of electron and hole transfer steps gives rise to characteristic cross-peak dynamics in the electronic 2D spectra, and we monitor how the excited state charge density ultimately localizes on the macrocycle closest to the counter-ion within 100 fs. A comparison with the dynamics in the radical species further elucidates how CT states modulate the electronic structure and tune fs-reaction dynamics. Our experiments demonstrate the unique capability of 2D-ES in combination with other methods to decipher ultrafast CT dynamics." @default.
- W2056146543 created "2016-06-24" @default.
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- W2056146543 date "2012-05-24" @default.
- W2056146543 modified "2023-09-27" @default.
- W2056146543 title "Ultrafast photo-induced charge transfer unveiled by two-dimensional electronic spectroscopy" @default.
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- W2056146543 doi "https://doi.org/10.1063/1.4720492" @default.
- W2056146543 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/22667567" @default.
- W2056146543 hasPublicationYear "2012" @default.
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