The blistering of elastic membranes is prone to elastic-solid as well as substrate-based mechanical instabilities. The solid-based instabilities have been well-explored in the mechanically indented blisters of elastic membranes over the rigid/ solid substrates, but an integrated study illustrating the underlying mechanism for the onset of solid as well as substrate-based instabilities in the spontaneous blistering of a 2D material is still lacking in the literature. In this article, an extensive experimental as well as analytical analysis of the spontaneous blister-formation in the multilayer graphene (MLG) flakes over a polymeric substrate is reported, which elucidates the involved mechanism and the governing parameters behind the development of elastic-solid as well as viscoelastic-substrate based instabilities. Herein, a ‘blister-collapse model’ is proposed, which infers that the suppression of the hoop compression, resulting from the phase-transition of the confined matter, plays a crucial role in the development of the instabilities. The ratio of blister-height to flake-thickness is a direct consequence of the taper-angle of the MLG blisters and the thickness-dependent elasticity of the upper-bounding MLG flakes, which shows a significant impact on the growth-dynamics of the viscous fingering patterns (viscoelastic-substrate based instabilities) under the MLG blisters.

The local or global straining techniques are used to modulate the electronic, vibrational and optical properties of the two-dimensional (2D) materials. However, manipulating the physical properties of a 2D material under a local strain is comparatively more challenging. In this work, we demonstrate an easy and efficient polymer curing assisted technique for the formation of optically visible multilayer Graphene (MLG) blisters of different shapes and sizes. The detailed spectroscopic and morphological analyses have been employed for exploring the dynamics of the confined matter inside the sub-micron blisters, which confirms that the confined matter inside the blister is liquid (water). From further analyses, we find the nonlinear elastic plate model as an acceptable model under certain limits for the mechanical analyses of the MLG blisters over the (poly)vinyl alcohol (PVA) polymer film to estimate the MLG-substrate interfacial adhesion energy and confinement pressure inside the blisters. The findings open new pathways for exploiting the technique for the formation of sub-micron blisters of the 2D materials for local strain-engineering applications, as well as the temperature-controlled release of the confined matter.

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