Second-order optical nonlinearities can be greatly enhanced by orders of magnitude in resonantly excited nanostructures. These resonant nonlinearities continually attract attention, particularly in newly discovered materials. However, they are frequently not as heightened as currently predicted, limiting their exploitation in nanostructured nonlinear optics. Here, we present a clear-cut theoretical and experimental demonstration that the second-order nonlinear susceptibility can vary by orders of magnitude as a result of giant destructive, as well as constructive, interference effects in complex systems. Using terahertz quantum cascade lasers as a model source to investigate interband and intersubband nonlinearities, we show that these giant interferences are a result of an unexpected interplay of the second-order nonlinear contributions of multiple light and heavy hole states. As well as of importance to understand and engineer the resonant optical properties of nanostructures, this advanced framework can be used as a novel, sensitive tool to elucidate the band structure properties of complex materials.
Substrate-emitting quantum cascade lasers with a distributed Bragg reflector and a spectrally detuned second-order outcoupler