TY - JOUR A1 - Sung, Jooyoung A1 - Kim, Pyosang A1 - Fimmel, Benjamin A1 - Würthner, Frank A1 - Kim, Dongho T1 - Direct observation of ultrafast coherent exciton dynamics in helical π-stacks of self-assembled perylene bisimides T2 - Nature Communications N2 - Ever since the discovery of dye self-assemblies in nature, there have been tremendous efforts to exploit biomimetic supramolecular assemblies for tailored artificial photon processing materials. This feature necessarily has resulted in an increasing demand for understanding exciton dynamics in the dye self-assemblies. In a sharp contrast with pi-type aggregates, however, the detailed observation of exciton dynamics in H-type aggregates has remained challenging. In this study, as we succeed in measuring transient fluorescence from Frenkel state of π-stacked perylene tetracarboxylic acid bisimide dimer and oligomer aggregates, we present an experimental demonstration on Frenkel exciton dynamics of archetypal columnar π-π stacks of dyes. The analysis of the vibronic peak ratio of the transient fluorescence spectra reveals that unlike the simple π-stacked dimer, the photoexcitation energy in the columnar π-stacked oligomer aggregates is initially delocalized over at least three molecular units and moves coherently along the chain in tens of femtoseconds, preceding excimer formation process. KW - systems KW - molecules KW - J-aggregate behavior KW - absorption KW - spectroscopy KW - photoluminescence KW - diffusion KW - fluorescence KW - excimer formation KW - organic semiconductors Y1 - 2015 UR - https://opus.bibliothek.uni-wuerzburg.de/frontdoor/index/index/docId/14815 UR - https://nbn-resolving.org/urn:nbn:de:bvb:20-opus-148157 VL - 6 IS - 8646 ER -