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J Chem Phys. 2013 May 14;138(18):184508. doi: 10.1063/1.4804398.

Two-photon-induced singlet fission in rubrene single crystal.

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  • 1Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore 637371, Singapore.


The two-photon-induced singlet fission was observed in rubrene single crystal and studied by use of femtosecond pump-probe spectroscopy. The location of two-photon excited states was obtained from the nondegenerate two-photon absorption (TPA) spectrum. Time evolution of the two-photon-induced transient absorption spectra reveals the direct singlet fission from the two-photon excited states. The TPA absorption coefficient of rubrene single crystal is 52 cm∕GW at 740 nm, as obtained from Z-scan measurements. Quantum chemical calculations based on time-dependent density functional theory support our experimental data.

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