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 χ⁽²⁾ once an in-plane electric field is applied. χ⁽²⁾ can be electrically tuned from 0 to ∼10⁵ pm/V, 3 orders of magnitude larger than the widely used nonlinear crystal AgGaSe₂. We show that the unusually large χ⁽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 χ⁽²⁾, which corresponds to a tunable wavelength ranging from ∼2.6 to ∼3.1 μm 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