Published in

American Association for the Advancement of Science, Research, (2020), 2020

DOI: 10.34133/2020/9085782

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Structuring Nonlinear Wavefront Emitted from Monolayer Transition-Metal Dichalcogenides

This paper is made freely available by the publisher.
This paper is made freely available by the publisher.

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Abstract

The growing demand for tailored nonlinearity calls for a structure with unusual phase discontinuity that allows the realization of nonlinear optical chirality, holographic imaging, and nonlinear wavefront control. Transition-metal dichalcogenide (TMDC) monolayers offer giant optical nonlinearity within a few-angstrom thickness, but limitations in optical absorption and domain size impose restriction on wavefront control of nonlinear emissions using classical light sources. In contrast, noble metal-based plasmonic nanosieves support giant field enhancements and precise nonlinear phase control, with hundred-nanometer pixel-level resolution; however, they suffer from intrinsically weak nonlinear susceptibility. Here, we report a multifunctional nonlinear interface by integrating TMDC monolayers with plasmonic nanosieves, yielding drastically different nonlinear functionalities that cannot be accessed by either constituent. Such a hybrid nonlinear interface allows second-harmonic (SH) orbital angular momentum (OAM) generation, beam steering, versatile polarization control, and holograms, with an effective SH nonlinearity χ 2 of ~25 nm/V. This designer platform synergizes the TMDC monolayer and plasmonic nanosieves to empower tunable geometric phases and large field enhancement, paving the way toward multifunctional and ultracompact nonlinear optical devices.