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We experimentally show that the rate of singlet fission in tetracene filmshas a superlinear dependence on the density of photo-excited singlet excitonswith ultrafast transient absorption spectroscopy. The spectrotemporal featuresof singlet and triplet dynamics can be disentangled from experimental data withthe algorithm of singular value decomposition. The correlation between theirtemporal dynamics indicates a nonlinear density dependence of fission rate,which leads to a conjecture of coherent singlet fission process arising fromsuperradiant excitons in crystalline tetracene. This hypothesis might be ableto resolve some long-standing controversies.

Superlinear density dependence of singlet fission rate in tetracene films