“…The freestanding membrane can be firmly “stuck” to the surface of any substratee.g., wafer, paper, plastic, etc.within the water, as fully demonstrated in Supporting Information, Video 1. It is interesting to note that this nonlayered PtS thin film can be spontaneously delaminated despite the absence of vdW physical gaps at its interface with the growth wafer, unlike the cases of vdW 2D TMD layers. ,− The working principle for this delamination phenomenon is believed to be an interplay of the water-driven exertion of a capillary force and the intrinsic surface wettability of the PtS thin film; i.e., the driving force, F , for the delamination of an as-grown thin film exposed to water is governed by the water surface tension capillary force, γ, and the water contact angle (WCA), θ, as in the equation F = γ (1 – cos θ). − This analysis leads to two conclusions; (1) films with higher hydrophobicity (i.e., a larger value for θ, a larger value for γ) are more prone to spontaneous delamination due to a stronger driving force (i.e., a larger value for F ), and (2) delamination efficacy can be controlled within the same sample by selectively adjusting its surface wettabilityi.e., spatially controlled value for θ. The distinct delamination characteristics of the PtS thin film determined by its surface hydrophobicity are illustrated in Supporting Information Figure S2.…”