Quantum-Enhanced Tunable Second-Order Optical Nonlinearity in Bilayer Graphene

Second order optical nonlinear processes involve the coherent mixing of two electromagnetic waves to generate a new optical frequency, which plays a central role in a variety of applications, such as ultrafast laser systems, rectifiers, modulators, and optical imaging. However, progress is limited in the mid-infrared (MIR) region due to the lack of suitable nonlinear materials. It is desirable to develop a robust system with a strong, electrically tunable second order optical nonlinearity. Here, we demonstrate theoretically that AB-stacked bilayer graphene (BLG) can exhibit a giant and tunable second order nonlinear susceptibility chi((2)) once an in-plane electric field is applied. chi((2)) can be electrically tuned from 0 to similar to 10(5) pm/V, 3 orders of magnitude larger than the widely used nonlinear crystal AgGaSe2. We show that the unusually large chi((2)) arise from two different quantum enhanced two-photon processes thanks to the unique electronic spectrum of BLG. The tunable electronic bandgap of BLG adds additional tunability on the resonance of chi((2)), which corresponds to a tunable wavelength ranging from similar to 2.6 to similar to 3.1 mu m for the up-converted photon. Combined with the high electron mobility and optical transparency of the atomically thin BLG, our scheme suggests a new regime of nonlinear photonics based on BLG.