Journal article

The role of conformational heterogeneity in the excited state dynamics of linked diketopyrrolopyrrole dimers dagger

Siobhan J Bradley, Ming Chi, Jonathan M White, Christopher R Hall, Lars Goerigk, Trevor A Smith, Kenneth P Ghiggino

PHYSICAL CHEMISTRY CHEMICAL PHYSICS | ROYAL SOC CHEMISTRY | Published : 2021

Abstract

Diketopyrrolopyrrole (DPP) derivatives have been proposed for both singlet fission and energy upconversion as they meet the energetic requirements and exhibit superior photostability compared to many other chromophores. In this study, both time-resolved electronic and IR spectroscopy have been applied to investigate excited state relaxation processes competing with fission in dimers of DPP derivatives with varying linker structures. A charge-separated (CS) state is shown to be an important intermediate with dynamics that are both solvent and linker dependent. The CS state is found for a subset of the total population of excited molecules and it is proposed that CS state formation requires su..

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Grants

Awarded by National Computational Merit Allocation Scheme


Awarded by Research Platform Services (ResPlat) at The University of Melbourne


Awarded by Australian Research Council through the Centre of Excellence in Exciton Science


Awarded by Australian Research Council


Funding Acknowledgements

The authors would like to thank Steve Meech, Greg Greetham, Ian Clark, James Iuliano and Jinnette Tolentino Collado for assistance with TIR measurements at the Rutherford Appleton Laboratory. L. G. acknowledges generous allocations of computational resources from the National Computational Infrastructure (NCI) Facility within the National Computational Merit Allocation Scheme (project fk5), and Research Platform Services (ResPlat) at The University of Melbourne (project punim0094). This work was supported by the Australian Research Council through the Centre of Excellence in Exciton Science (CE170100026) and grant LE200100051.