Interlayer exciton mediated second harmonic generation in bilayer MoS2

Shivangi Shree, Delphine Lagarde, Laurent Lombez, Cedric Robert, Andrea Balocchi, Kenji Watanabe, Takashi Taniguchi, Xavier Marie, Iann C. Gerber, Mikhail M. Glazov (), Leonid E. Golub, Bernhard Urbaszek () and Ioannis Paradisanos ()
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Shivangi Shree: Université de Toulouse, INSA-CNRS-UPS, LPCNO
Delphine Lagarde: Université de Toulouse, INSA-CNRS-UPS, LPCNO
Laurent Lombez: Université de Toulouse, INSA-CNRS-UPS, LPCNO
Cedric Robert: Université de Toulouse, INSA-CNRS-UPS, LPCNO
Andrea Balocchi: Université de Toulouse, INSA-CNRS-UPS, LPCNO
Kenji Watanabe: Research Center for Functional Materials, National Institute for Materials Science
Takashi Taniguchi: International Center for Materials Nanoarchitectonics, National Institute for Materials Science
Xavier Marie: Université de Toulouse, INSA-CNRS-UPS, LPCNO
Iann C. Gerber: Université de Toulouse, INSA-CNRS-UPS, LPCNO
Mikhail M. Glazov: Ioffe Institute
Leonid E. Golub: Ioffe Institute
Bernhard Urbaszek: Université de Toulouse, INSA-CNRS-UPS, LPCNO
Ioannis Paradisanos: Université de Toulouse, INSA-CNRS-UPS, LPCNO

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract 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.

Date: 2021
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DOI: 10.1038/s41467-021-27213-8

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