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

preprint
submitted on 24.07.2020, 20:40 and posted on 28.07.2020, 13:08 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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