Inverse Design of Tetracene Polymorphs with Enhanced Singlet Fission Performance by Property-Based Genetic Algorithm Optimization

0568115 - ÚOCHB 2024 RIV US eng J - Journal Article
Tom, R. - Gao, S. - Yang, Y. - Zhao, K. - Bier, I. - Buchanan, E. A. - Zaykov, Alexandr - Havlas, Zdeněk - Michl, Josef - Marom, N.
Inverse Design of Tetracene Polymorphs with Enhanced Singlet Fission Performance by Property-Based Genetic Algorithm Optimization.
Chemistry of Materials. Roč. 35, č. 3 (2023), s. 1373-1386. ISSN 0897-4756. E-ISSN 1520-5002
Research Infrastructure: e-INFRA CZ - 90140
Institutional support: RVO:61388963
Keywords : crystal structure prediction * exciton fission * thin film
OECD category: Physical chemistry
Impact factor: 8.6, year: 2022
Method of publishing: Open access
https://doi.org/10.1021/acs.chemmater.2c03444

The efficiency of solar cells may be improved by using singlet fission (SF), in which one singlet exciton splits into two triplet excitons. SF occurs in molecular crystals. A molecule may crystallize in more than one form, a phenomenon known as polymorphism. Crystal structure may affect SF performance. In the common form of tetracene, SF is experimentally known to be slightly endoergic. A second, metastable polymorph of tetracene has been found to exhibit better SF performance. Here, we conduct inverse design of the crystal packing of tetracene using a genetic algorithm (GA) with a fitness function tailored to simultaneously optimize the SF rate and the lattice energy. The property-based GA successfully generates more structures predicted to have higher SF rates and provides insight into packing motifs associated with improved SF performance. We find a putative polymorph predicted to have superior SF performance to the two forms of tetracene, whose structures have been determined experimentally. The putatuve structure has a lattice energy within 1.5 kJ/mol of the most stable common form of tetracene.
Permanent Link: https://hdl.handle.net/11104/0339456