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 putative structure has a lattice energy within 1.5 kJ/mol of the most stable common form of tetracene.

Department of Chemistry Carnegie Mellon University Pittsburgh Pennsylvania15213 United States

Department of Chemistry University of Colorado Boulder Colorado80309 United States

Department of Materials Science and Engineering Carnegie Mellon University Pittsburgh Pennsylvania15213 United States

Department of Physical Chemistry University of Chemistry and Technology 166 28Prague 6 Czech Republic

Department of Physics Carnegie Mellon University Pittsburgh Pennsylvania15213 United States

Institute of Organic Chemistry and Biochemistry Czech Academy of Sciences 16610Prague 6 Czech Republic

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The seventh blind test of crystal structure prediction: structure ranking methods