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The contact between two rough surfaces has been a topic of significant interest since early studies on Coulombic friction and remains crucial for numerous technological applications. However, theoretical progress has outpaced experiments due to the challenges in measuring contact areas across scales ranging from subnanometers to macroscopic dimensions. Here, we demonstrate the use of commonly available infrared-based (IR) spectroscopy in combination with finite-difference time-domain (FDTD) optical simulations to measure separation gaps and contact areas for glassy polymers ranging in roughness over two orders in magnitude. With the combined IR and FDTD simulations, we can overcome the optical diffraction limits and take advantage of the chemical specificity of IR spectroscopy to overcome limitations due to scattering. The scaling of the contact area ratio as a function of pressure illustrated the limitations of using pure elastic or plastic deformation in explaining the results. At both low and high pressures, the contact area ratios scale linearly with pressure as expected for purely elastic deformations at low pressures or plastic deformations at high pressures. However, if analyzed over a broad range of pressure, the power laws we observe are much larger than 1, exemplifying the need to consider elastoplastic models in explaining results for softer polymer contacts compared to other brittle, glassy materials. In comparison, the separation gaps scale exponentially with pressure, as expected. These results have important implications for the interpretation of properties such as friction, adhesion, and conductivity for softer, glassy contact interfaces. 

Adhesives require molecular contact, which is governed by roughness, modulus, and load. Here, we measured adhesion for stiff glassy polymer layers of varying thickness on top of a soft elastomer with rough substrates. We found that a 90-nm-thick PMMA layer on a softer elastic block was sufficient to drop macroscopic adhesion to almost zero during the loading cycle. This drop in adhesion for bilayers follows the modified Persson-Tosatti model, where the elastic energy for conformal contact depends on the thickness and modulus of the bilayer. In contrast, we observed no dependence on thickness of the PMMA layer on the work of adhesion calculated using the pull-off forces. Understanding how mechanical gradients (like bilayers) affect adhesion is critical for areas such as adhesion, friction, and colloidal and granular physics. Published by the American Physical Society2024