Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 5, Issue 20, Pages 3601-3607Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jz501953a
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Funding
- Midcareer Researcher Program - Ministry of Education, Science and Technology (MEST) [2005-0093839]
- Deutsche Forschungsgemeinschaft within research graduate school [GK 1221]
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Although it is commonly known that H-type PBI aggregates give rise to a broad, red-shifted excimer fluorescence with considerably longer fluorescence lifetimes than observed for the monomers, the underlying mechanisms of excimer formation and other relevant exciton dynamics in such pi-stacked systems are still far from being understood. In this context, we demonstrate a thorough spectroscopic investigation on the exciton relaxation pathways, including excimer formation, in a perylene-3,4:9,10-bis(dicarboximide) (PBI) dimer aggregate 1 by using time-resolved fluorescence and transient absorption spectroscopy combined with excitation-power and polarization dependence. It was found that the excited dimer formation process followed by structural rearrangement is approximately two times faster than observed within larger PBI aggregates. Excitation-power-dependent transient absorption decay profiles revealed the fully delocalized nature of excitons in the dimer as opposed to larger stacks.
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