Superlinear density dependence of singlet fission rate in tetracene films

Abstract

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

arXiv comment20 pages, 4 figures, together with Supplementary Information

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• Polarized superradiance from delocalized exciton transitions in tetracene single crystals
• Competition between the Pseudogap and Superconducting States of Bi${}_2$Sr${}_2$Ca${}_{0.92}$Y${}_{0.08}$Cu${}_2$O${}_{8+\delta }$ Single Crystals Revealed by Ultrafast Broadband Optical Reflectivity
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Cited by in corpus (5)

• Magnetic dipolar interaction between correlated triplets created by singlet fission in tetracene crystals
• Coherent dynamics of singlet fission controlled by nonlocal electron-phonon coupling
• Polarization-dependent exciton dynamics in tetracene single crystals
• Beating maps of singlet fission: Full-quantum simulation of coherent two-dimensional electronic spectroscopy in organic aggregates
• The anomalous process in singlet fission kinetic model with time-dependent coefficient