Engineering nonlinear response of nanomaterials using Fano resonances

We show that nonlinear optical processes of nanoparticles can be controlled by the presence of interactions with a molecule or a quantum dot. By choosing the appropriate level spacing for the quantum emitter, one can either suppress or enhance the nonlinear frequency conversion. We reveal the underlying mechanism for this effect, which is already observed in recent experiments: (i) suppression occurs simply because transparency induced by Fano resonance does not allow an excitation at the converted frequency, and (ii) enhancement emerges since the nonlinear process can be brought to resonance. The path interference effect cancels the nonresonant frequency terms. We demonstrate the underlying physics using a simplified model, and we show that the predictions of the model are in good agreement with the three-dimensional boundary element method (MNPBEM toolbox) simulations. Here, we consider the second harmonic generation in a plasmonic converter as an example to demonstrate the control mechanism. The phenomenon is the semi-classical analog of nonlinearity enhancement via electromagnetically induced transparency. (paper)