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Controlling Singlet Fission with Coordination Chemistry-Induced Assembly of Dipyridyl Pyrrole Bipentacenes

preprint
submitted on 24.07.2020 and posted on 28.07.2020 by Ryan Ribson, Gyeongshin Choi, Ryan Hadt, Theodor Agapie
Singlet fission has the potential to surpass current efficiency limits in next-generation photovoltaics and to find use in quantum information science. Despite the demonstration of singlet fission in various materials, there is still a great need for fundamental design principles that allow for tuning of photophysical parameters, including the rate of fission and triplet lifetimes. Here we describe the synthesis and photophysical characterization of a novel bipentacene dipyridyl pyrrole (HDPP-Pent) and its Li- and K-coordinated derivatives. HDPP-Pent undergoes singlet fission at roughly 50% efficiency (τSF = 730 ps), whereas coordination in the Li complex induces significant structural changes to generate a dimer, resulting in a 5-fold rate increase (τSF = 140 ps) and near fully efficient singlet fission with virtually no sacrifice in triplet lifetime. We thus illustrate novel design principles to produce favorable singlet fission properties, wherein through-space control can be achieved via coordination chemistry-induced multi-pentacene assembly.

History

Email Address of Submitting Author

rghadt@caltech.edu

Institution

California Institute of Technology

Country

United States

ORCID For Submitting Author

0000-0001-6026-1358

Declaration of Conflict of Interest

No conflict of interest

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