@article{SungKimFimmeletal.2015, author = {Sung, Jooyoung and Kim, Pyosang and Fimmel, Benjamin and W{\"u}rthner, Frank and Kim, Dongho}, title = {Direct observation of ultrafast coherent exciton dynamics in helical π-stacks of self-assembled perylene bisimides}, series = {Nature Communications}, volume = {6}, journal = {Nature Communications}, number = {8646}, doi = {10.1038/ncomms9646}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-148157}, year = {2015}, abstract = {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.}, language = {en} } @article{HongKimKimetal.2022, author = {Hong, Yongseok and Kim, Woojae and Kim, Taeyeon and Kaufmann, Christina and Kim, Hyungjun and W{\"u}rthner, Frank and Kim, Dongho}, title = {Real-time Observation of Structural Dynamics Triggering Excimer Formation in a Perylene Bisimide Folda-dimer by Ultrafast Time-Domain Raman Spectroscopy}, series = {Angewandte Chemie International Edition}, volume = {61}, journal = {Angewandte Chemie International Edition}, number = {13}, doi = {10.1002/anie.202114474}, url = {http://nbn-resolving.de/urn:nbn:de:bvb:20-opus-318788}, year = {2022}, abstract = {In π-conjugated organic photovoltaic materials, an excimer state has been generally regarded as a trap state which hinders efficient excitation energy transport. But despite wide investigations of the excimer for overcoming the undesirable energy loss, the understanding of the relationship between the structure of the excimer in stacked organic compounds and its properties remains elusive. Here, we present the landscape of structural dynamics from the excimer formation to its relaxation in a co-facially stacked archetypical perylene bisimide folda-dimer using ultrafast time-domain Raman spectroscopy. We directly captured vibrational snapshots illustrating the ultrafast structural evolution triggering the excimer formation along the interchromophore coordinate on the complex excited-state potential surfaces and following evolution into a relaxed excimer state. Not only does this work showcase the ultrafast structural dynamics necessary for the excimer formation and control of excimer characteristics but also provides important criteria for designing the π-conjugated organic molecules.}, language = {en} }