Spectroscopic Determination of Ice‐Induced Interfacial Strain on Single‐Layer Graphene

Abstract Reliably determining the physical properties of ice (e.g., crystal structure, adhesion strength, interfacial state, and molecular orientation) has proven to be both challenging and highly dependent on experiment‐specific conditions, including surface roughness, ice formation, water purity, and measurement method. Here, non‐destructive measurements of single‐layer graphene (SLG) interfaced with bulk ice are used to determine temperature‐dependent, ice‐induced strain and estimate ice‐created strain elastic density in SLG. The use of SLG enables the precise study of interfacial strain by monitoring the 2D Raman mode. Upon ice formation, a clear, ≈2 cm⁻¹ decrease in the 2D mode frequency is observed, which is ascribed to a 0.012% biaxial tensile shear strain at the ice–SLG interface. From this shear strain value, the ice‐created SLG elastic strain energy density is estimated to be 2.4 μJ m⁻². In addition to these Raman strain measurements, intentionally ionized water is used to show that water‐mediated charging of the SLG surface manifests itself in a distinctly different manner than ice‐induced strain. Finally, the localized nature of the Raman probe is used to map SLG regions with and without ice, suggesting that this method cannot only determine ice‐induced interfacial strain, but also correlate ice adhesion properties with surface roughness and topology.