期刊
JOURNAL OF CHEMICAL PHYSICS
卷 136, 期 20, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.4720492
关键词
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资金
- Austrian Science Foundation (FWF) [P223311, F016-18]
- sterreichischer Austauschdienst (OeAD) [WTZ CZ07/2011]
- Deutsche Forschungsgemeinschaft through the DFG-Cluster of Excellence Munich-Centre for Advanced Photonics
- Czech Science Foundation (GACR) [205/10/0989]
- Ministry of Education, Youth, and Sports of the Czech Republic [KONTAKT ME899, MSM0021620835]
- Wenner-Gren foundation
- Austrian Science Fund (FWF) [P 22331] Funding Source: researchfish
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. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4720492]
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