Highly Stretchable and Transparent Optical Adhesive Films Using Hierarchically Structured Rigid-Flexible Dual-Stiffness Nanoparticles

The demand for new forms of flexible electronic devices has led to the evolution of individual components comprising optical adhesive films that provide excellent optical transparency and high bonding strength while offering remarkable elasticity with high strain and recovery properties. Herein, a new type of highly elastic and transparent adhesive film is proposed using tailored rigid-flexible dual-stiffness nanoparticles (DSNs) composed of a rigid inorganic core and an elastic reactive coil shell. The hierarchically structured nanoparticles were prepared from SiO₂ nanoparticles via the sequential surface modification with photoreactive flexible chains. The fabricated elastic adhesive film containing DSNs with an average diameter of 20 nm showed a high optical transmittance of 92% and adhesion strength of 19.9 N/25 mm. Increasing the content of the tailored nanoparticles in the adhesive film improved the elastic properties of the film such as elastic modulus (7.0 kPa), stress relaxation ratio (18.4%), and strain recovery rate (73.6%) due to the efficient elastic motion of the embedded DSNs. In addition, as the surface grafting density of elastic coil groups in the nanoparticle increased, a stronger bonding network was formed between the nanoparticles and the acrylic polymer matrix, thereby further improving the stress relaxation ratio (18.0%) and strain recovery rate (77.1%) of the optical film. Thus, the utilization of novel dual-stiffness nanoparticles produces optical adhesive films with high elasticity and optical transparency that are capable of withstanding external forces such as folding and stretching, which is essential for flexible electronic devices.