Interlayer exciton mediated second harmonic generation in bilayer MoS2.

Second-harmonic generation (SHG) is a non-linear optical process, where two photons coherently combine into one photon of twice their energy. Efficient SHG occurs for crystals with broken inversion symmetry, such as transition metal dichalcogenide monolayers. Here we show tuning of non-linear optical processes in an inversion symmetric crystal. This tunability is based on the unique properties of bilayer MoS2, that shows strong optical oscillator strength for the intra- but also interlayer exciton resonances. As we tune the SHG signal onto these resonances by varying the laser energy, the SHG amplitude is enhanced by several orders of magnitude. In the resonant case the bilayer SHG signal reaches amplitudes comparable to the off-resonant signal from a monolayer. In applied electric fields the interlayer exciton energies can be tuned due to their in-built electric dipole via the Stark effect. As a result the interlayer exciton degeneracy is lifted and the bilayer SHG response is further enhanced by an additional two orders of magnitude, well reproduced by our model calculations. Since interlayer exciton transitions are highly tunable also by choosing twist angle and material combination our results open up new approaches for designing the SHG response of layered materials.

Terahertz Photogalvanics in Twisted Bilayer Graphene Close to the Second Magic Angle.

We report on the observation of photogalvanic effects in tBLG with a twist angle of 0.6°. We show that excitation of the tBLG bulk causes a photocurrent, whose sign and magnitude are controlled by the orientation of the radiation electric field and the photon helicity. The observed photocurrent provides evidence for the reduction of the point group symmetry in low twist-angle tBLG to the lowest possible one. The developed theory shows that the current is formed by asymmetric scattering in gyrotropic tBLG. We also detected the photogalvanic current formed in the vicinity of the edges. For both bulk and edge photocurrents, we demonstrate the emergence of pronounced oscillations upon variation of the gate voltage. The gate voltages associated with the oscillations correlate with peaks in resistance measurements. These are well explained by interband transitions between a multitude of isolated bands in tBLG.