Vibronic and excitonic dynamics in perylenediimide dimers and tetramer

Ivo H.M. Van Stokkum*, Chanelle C. Jumper, Tia S. Lee, Mykhaylo Myahkostupov, Felix N. Castellano, Gregory D. Scholes

*Corresponding author for this work

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Abstract

Broad-band pump-probe spectroscopy combined with global and target analysis is employed to study the vibronic and excitonic dynamics of two dimers and a tetramer of perylenediimides. A simultaneous analysis is developed for two systems that have been measured in the same conditions. This enhances the resolvability of the vibronic and excitonic dynamics of the systems, and the solvent contributions that are common in the experiments. We resolve two oscillations of 1399 cm-1 or 311 cm-1 damped with ≈30/ps involved in vibrational relaxation and two more oscillations of 537 cm-1 or 136 cm-1 damped with ≈3/ps. A relaxation process with a rate of 2.1/ps-3.2/ps that is positively correlated with the excitonic coupling was discovered in all three model systems, attributed to annihilation of the one but lowest exciton state.

Original languageEnglish
Article number224101
Pages (from-to)1-10
Number of pages10
JournalJournal of Chemical Physics
Volume153
Issue number22
Early online date8 Dec 2020
DOIs
Publication statusPublished - 14 Dec 2020

Funding

This work was supported by the Natural Sciences and Engineering Research Council of Canada, DARPA (QuBE) and the United States Air Force Office of Scientific Research Contract No. FA9550-13-1-0005 to G.D.S. and by the research scholarship from the Natural Sciences and Engineering Research Council of Canada and the Ontario Graduate Scholarship to C.C.J. The NCSU portion of this work was supported by the Air Force Office of Scientific Research (Grant No. FA9550-18-1-0331).

FundersFunder number
United States Air Force Office of Scientific ResearchFA9550-13-1-0005
Air Force Office of Scientific ResearchFA9550-18-1-0331
Defense Advanced Research Projects Agency
Natural Sciences and Engineering Research Council of Canada

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