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Two-photon-induced singlet fission in rubrene single crystal
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Image of FIG. 1.
FIG. 1.

(a) Steady state absorption and fluorescence spectra of rubrene single crystal (inset: molecular structure). (b) TA spectra for rubrene single crystal after chirp correction, = 650 nm. The region 625–675 nm of strong scattered excitation light is removed. The upper and lower parts show the TA spectra at different time ranges.

Image of FIG. 2.
FIG. 2.

Transient kinetics at 444 nm and 510 nm probe wavelengths. Inset shows the kinetics within the first 5 ps.

Image of FIG. 3.
FIG. 3.

Log-log plot of TA signal at different delay times (0.2 and 50 ps) of rubrene crystal as a function of pumping power, = 650 nm. The inset shows the schematic of temporal positions at 550 nm probe chosen for the fast process.

Image of FIG. 4.
FIG. 4.

(a) Schematic of the transitions for one-photon absorption (OPA), nondegenerate two-photon absorption (ND-TPA), and degenerate two-photon absorption (D-TPA) processes. (b) OPA and ND-TPA spectra (under 650 and 750 nm pump).

Image of FIG. 5.
FIG. 5.

Normalized transient absorption kinetics at = 510 nm under OPA (250–550 nm) and TPA (650 nm). (Inset) Arrhenius plot of singlet fission rate versus pump photon energy.

Image of FIG. 6.
FIG. 6.

Rubrene molecule conformations in single crystal (a) and solution (b).


Generic image for table
Table I.

Global fit results for 510 nm transient kinetics under different pump wavelength ( ).


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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Two-photon-induced singlet fission in rubrene single crystal