In this paper, we show experimentally that for van der Waals heterostructures (vdWh) of atomically-thin materials, the hybridization of bands of adjacent layers is possible only for ultra-clean interfaces. This we achieve through a detailed experimental study of the effect of interfacial separation and adsorbate content on the photoluminescence emission and Raman spectra of ultra-thin vdWh. For vdWh with atomically-clean interfaces, we find the emergence of novel vibrational Raman-active modes whose optical signatures differ significantly from that of the constituent layers. Additionally, we find for such systems a significant modification of the photoluminescence emission spectra with the appearance of peaks whose strength and intensity directly correlate with the inter-layer coupling strength. Our ability to control the intensity of the photoluminescence emission led to the observation of detailed optical features like indirect-band peaks. Our study establishes that it is possible to engineer atomically-thin van der Waals heterostructures with desired optical properties by controlling the inter-layer spacing, and consequently the inter-layer coupling between the constituent layers.
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