2020, Ngo G.Q., George A., Schock R.T.K., Tuniz A., Najafidehaghani E., Gan Z., Geib N.C., Bucher T., Knopf H., Saravi S., Neumann C., Lühder T., Schartner E.P., Warren-Smith S.C., Ebendorff-Heidepriem H., Pertsch T., Schmidt M.A., Turchanin A., Eilenberger F.

Atomically thin transition metal dichalcogenides are highly promising for integrated optoelectronic and photonic systems due to their exciton-driven linear and nonlinear interactions with light. Integrating them into optical fibers yields novel opportunities in optical communication, remote sensing, and all-fiber optoelectronics. However, the scalable and reproducible deposition of high-quality monolayers on optical fibers is a challenge. Here, the chemical vapor deposition of monolayer MoS2 and WS2 crystals on the core of microstructured exposed-core optical fibers and their interaction with the fibers’ guided modes are reported. Two distinct application possibilities of 2D-functionalized waveguides to exemplify their potential are demonstrated. First, the excitonic 2D material photoluminescence is simultaneously excited and collected with the fiber modes, opening a novel route to remote sensing. Then it is shown that third-harmonic generation is modified by the highly localized nonlinear polarization of the monolayers, yielding a new avenue to tailor nonlinear optical processes in fibers. It is anticipated that the results may lead to significant advances in optical-fiber-based technologies. © 2020 The Authors. Published by Wiley-VCH GmbH