Nonlinear Dispersion Relation and Out-of-Plane Second Harmonic Generation in MoSSe and WSSe Janus Monolayers

Abstract

Janus transition metal dichalcogenides are an emerging class of atomically thin materials with engineered broken mirror symmetry that gives rise to long-lived dipolar excitons, Rashba splitting, and topologically protected solitons. They hold great promise as a versatile nonlinear optical platform due to their broadband harmonic generation tunability, ease of integration on photonic structures, and nonlinearities beyond the basal crystal plane. Here, we study second and third harmonic generation in MoSSe and WSSe Janus monolayers. We use polarization-resolved spectroscopy to map the full second-order susceptibility tensor of MoSSe, including its out-of-plane components. In addition, we measure the effective third-order susceptibility, and the second-order nonlinear dispersion close to exciton resonances for both MoSSe and WSSe at room and cryogenic temperatures. Our work sets a bedrock for understanding the nonlinear optical properties of Janus transition metal dichalcogenides and probing their use in the next-generation on-chip multifaceted photonic devices.

10 pages, 3 figures. SI: 8 pages, 5 figures

References in corpus (6)

• Non-linear Optical Spectroscopy of Excited Exciton States for Efficient Valley Coherence Generation in WSe2 Monolayers
• All-optical polarization and amplitude modulation of second-harmonic generation in atomically thin semiconductors
• Spectroscopic Signatures of Interlayer Coupling in Janus MoSSe/MoS2 Heterostructures
• Electrically Tunable Four-Wave-Mixing in Graphene Heterogeneous Fiber for Individual Gas Molecule Detection
• Parametric Nonlinear Optics with Layered Materials and Related Heterostructures
• A Monolithic Graphene-Functionalized Microlaser for Multispecies Gas Detection

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• Atomically-precise synthesis and simultaneous integration of 2D transition metal dichalcogenides enabled by nano-confinement