Raman Spectroscopic Probe for Nonlinear MoS Nanoelectromechanical Resonators.

Resonant nanoelectromechanical systems (NEMS) enabled by two-dimensional (2D) semiconductors have been actively explored and engineered for making ultrascaled transducers toward applications in ultralow-power signal processing, communication, and sensing. Although the transduction of miniscule resonant motions has been achieved by low-noise optical or electronic techniques, direct probing of strain in vibrating 2D semiconductor membranes and the interplay between the spectroscopic and mechanical properties are still largely unexplored. Here, we experimentally demonstrate dynamical phonon softening in atomically thin molybdenum disulfide (MoS) NEMS resonators by directly coupling Raman spectroscopy with optical interferometry resonance motion detection. In single-layer, bilayer, and trilayer (1L to 3L) MoS circular membrane NEMS resonators, we show that high-amplitude nonlinear resonances can enhance the Raman signal amplitude, as well as introduce Raman modes softening up to 0.8 cm. These results shall pave the way for engineering the coupling and control between collective mechanical vibrations and Raman modes of the constituent crystals in 2D transducers.