Organic–inorganic heterostructures for nonlinear optics

We consider a hybrid heterostructure made of an inorganic quantum well in close proximity with an organic material overlayer, whereby the latter is used to funnel excitation energy to the former in order to exploit the optical nonlinearities of the two-dimensional Wannier excitons. The resonant optical pumping of the Frenkel excitons and their diffusion to the organic–inorganic interface can lead to an efficient indirect pumping of the inorganic quantum well turning on the corresponding nonlinearities. As organic material we consider a layer of anthracene or of tetracene. In the latter case, the singlet exciton has an energy which is close to twice the one of a triplet exciton and singlet exciton fission into two triplets can be efficient. In tetracene based hybrid heterostructures, the temperature dependence of fission opens the possibility to turn on and off the indirect pumping due to energy transfer from the organic into the inorganic subsystem. Finally, we show how a generic mechanism of dipole–dipole hybridization may lead to the formation of virtual heterodimers of organic molecules with an enhanced nonlinear optical response. - Highlights: • Organic-inorganic heterostructures offer new possibilities for enhanced optoelectronic functionalities. • We show how an organic overlayer can harvest light and funnel excitation energy to an inorganic quantum well turning on its optical nonlinearities. • The illustrative cases of anthracene and tetracene overlayers are considered, the latter showing the important role of temperature dependent singlet exciton fission processes. • A generic model of hybrid dimers is discussed showing how optical nonlinearities might be enhanced both in the strong and weak coupling regimes.