Enhanced Interband Optical Nonlinearities from Coupled Quantum Wells

The recent, rapid advances in nonlinear chipscale nanophotonics in the visible and near-infrared have been largely driven by manipulating the local dielectric environment proximate to decades-old workhorse bulk nonlinear optical materials, rather than increasing the inherent strength of their nonlinear response. While proposed decades ago, we demonstrate the first experimental realization of a new class of designer nonlinear materials that leverage the interband optical transition in asymmetric structures to provide strong second order susceptibility, $\chi^{(2)}$. Using simple AlGaAs/GaAs coupled quantum wells operating in the near-infrared as a prototype, we observed strong second harmonic generation enhancement of 1550 nm to 775 nm over bulk controls. Extracted $\chi^{(2)}$ values were as high as 2750 pm/V, which is $>$7x that of bulk GaAs. Furthermore, measured susceptibilities agreed well with quantum mechanical calculations of $\chi^{(2)}$ using layer profiles extracted from electron microscopy. Growth interruptions were employed to improve interfacial abruptness in response to electron microscopy characterization, resulting in increased $\chi^{(2)}$ toward the simulation predictions for ideal heterointerfaces. More complex layer designs showed predicted $\chi^{(2)}$ up to 7 nm/V. Such materials are anticipated to find myriad applications, including entangled photon generation at telecommunications wavelengths for chipscale quantum information processing.