Strong and tunable interlayer coupling of infrared-active phonons to excitons in van der Waals heterostructures

Understanding and manipulating the quantum interlayer exciton-phonon coupling in van der Waals heterostructures, especially for infrared active phonons with electromagnetic fields, would set a foundation for realizing exotic quantum phenomena and optoelectronic applications. Here we report experimental observations of strong mutual interactions between infrared active phonons in hexagonal boron nitride (hBN) and excitons in WS2. Our results underscore that the infrared active A2u mode of hBN becomes Raman active with strong intensities in WS2/hBN heterostructures through resonant coupling to the B exciton of WS2. Moreover, we demonstrate that the activated A2u phonon of hBN can be tuned by the hBN thickness and harbors a striking anticorrelation intensity modulation, as compared with the optically silent B1g mode. Our observation of the interlayer exciton-infrared active phonon interactions and their evolution with hBN thickness provide a firm basis for engineering the hyperbolic exciton-phonon polaritons, chiral phonons and fascinating nanophotonics based on van der Waals heterostructures.