Large optical nonlinearity induced by singlet fission in pentacene films

Angew Chem Int Ed Engl. 2015 May 18;54(21):6222-6. doi: 10.1002/anie.201501396. Epub 2015 Apr 2.

Abstract

By creating two triplet excitons from one photo-excited singlet exciton, singlet fission in organic semiconductors has drawn tremendous attention for its potential applications in boosting the efficiency of solar conversion. Here, we show that this carrier-multiplication effect can also be used to dramatically improve the nonlinear optical response in organic materials. We have observed large optical nonlinearity with a magnitude of χ((3)) up to 10(-9) esu in pentacene films, which is further shown to be a result of singlet fission by monitoring the temporal dynamics. The potential application of such efficient nonlinear optical response has been demonstrated with a singlet-fission-induced polarization rotation.

Keywords: nonlinear optics; pentacene; singlet fission; time-resolved spectroscopy.