Giant enhancement of optical nonlinearity in two-dimensional materials by multiphoton-excitation resonance energy transfer from quantum dots

Colloidal quantum dots are promising photoactive materials that enable plentiful photonic and optoelectronic applications ranging from lasers, displays and photodetectors to solar cells^1–9. However, these applications mainly utilize the linear optical properties of quantum dots, and their great potential in the broad nonlinear optical regime is still waiting for full exploration^10–12. Here, we demonstrate that a simple coating of a sub-200-nm-thick quantum dot film on two-dimensional materials can significantly enhance their nonlinear optical responses (second, third and fourth harmonic generation) by more than three orders of magnitude. Systematic experimental results indicate that this enhancement is driven by a non-trivial mechanism of multiphoton-excitation resonance energy transfer, where the quantum dots directly deliver their strongly absorbed multiphoton energy to the adjacent two-dimensional materials by a remote dipole–dipole coupling. Our findings could expand the applications of quantum dots in many exciting areas beyond linear optics, such as nonlinear optical signal processing, multiphoton imaging and ultracompact nonlinear optical elements.