We report on the observation of two hypersonic phononic gaps of different nature in three-dimensional colloidal films of nanospheres using Brillouin light scattering. One is a Bragg gap occurring at the edge of the first Brillouin zone along a high-symmetry crystal direction. The other is a hybridization gap in crystalline and amorphous films, originating from the interaction of the band of quadrupole particle eigenmodes with the acoustic effective-medium band, and its frequency position compares well with the computed lowest eigenfrequency. Structural disorder eliminates the Bragg gap, while the hybridization gap is robust.
The design and engineering of hybrid materials exhibiting tailored phononic band gaps are fundamentally relevant to innovative material technologies in areas ranging from acoustics to thermo-optic devices. Phononic hybridization gaps, originating from the anti-crossing between local resonant and propagating modes, have attracted particular interest because of their relative robustness to structural disorder and the associated benefit to ‘manufacturability'. Although hybridization gap materials are well known, their economic fabrication and efficient control of the gap frequency have remained elusive because of the limited property variability and expensive fabrication methodologies. Here we report a new strategy to realize hybridization gap materials by harnessing the ‘anisotropic elasticity' across the particle–polymer interface in densely polymer-tethered colloidal particles. Theoretical and Brillouin scattering analysis confirm both the robustness to disorder and the tunability of the resulting hybridization gap and provide guidelines for the economic synthesis of new materials with deliberately controlled gap position and width frequencies.
The present work demonstrates the first application of Brillouin light scattering (BLS) to probe film-guided elastic waves in transparent-substrate supported polymer thin films. In comparison with earlier BLS studies that were restricted to films either free-standing or supported on opaque substrates, the progress made in this work substantially extends the applicability of BLS and permits direct access to the elastic properties of thin films lying on transparent substrates, which is of important practical relevance. A series of thin supported polystyrene and poly(methyl methacrylate) films with thickness in the range of 40-500 nm were explored, and no noticeable trend in elastic properties with thickness has been found, in conformity with earlier BLS results. The first measurement of glass transition temperature, T g , of supported polymer thin films by BLS is also reported. We observed that the ultrathin (40 nm) films for both polymers exhibit a clear reduction in T g .
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