Profiles in the local glass transition temperature T g(z) within polystyrene (PS) next to polydimethylsiloxane (PDMS) domains were determined using a localized fluorescence method. By changing the base to cross-linker ratio, we varied the cross-link density and, hence, the Young’s modulus of PDMS (Sylgard 184). The local T g(z) in PS at a distance of z = 50 nm away from the PS/PDMS interface was found to shift by 40 K as the PDMS modulus was varied from 0.9 to 2.6 MPa, demonstrating a strong sensitivity of this phenomenon to the rigidity of the neighboring domain. The extent the T g(z) perturbation persists away from the PS/PDMS interface, z ≈ 65–90 nm before bulk T g is recovered, is much shorter for this strongly immiscible system compared with the weakly immiscible systems studied previously, which we attribute to a smaller interfacial width, as the χ parameter for PS/PDMS is an order of magnitude larger.

Employing a quartz crystal microbalance (QCM) as a MHz‐viscoelastic sensor requires extracting information from higher harmonics beyond the Sauerbrey limit, which can be problematic for rubbery polymer films that are highly dissipative because of the onset of anharmonic side bands and film resonance. Data analysis for QCM can frequently obscure the underlying physics or involve approximations that tend to break down at higher harmonics. In this study, modern computational tools are leveraged to solve a continuum physics model for the QCM's acoustic shear wave propagation through a polymer film with zero approximations, retaining the physical intuition of how the experimental signal connects to the shear modulus of the material. The resulting set of three coupled equations are solved numerically to fit experimental data for the resonance frequency Δfn and dissipation ΔΓn shifts as a function of harmonic number n, over an extended harmonic range approaching film resonance. This allows the frequency‐dependent modulus of polymer films at MHz frequencies, modeled as linear on a log–log scale, to be determined for rubbery polybutadiene (PB) and polydimethylsiloxane (PDMS) films, showing excellent agreement with time–temperature shifted rheometry data from the literature.