Symmetry in photonic crystals is reflected in the structure of their photonic bands and symmetry breaking can result in the development of complete photonic band gaps, leading to enhanced optical properties. This can be difficult for self-assembled nanostructures, due to their restriction by fundamental principles to preferential geometries, but can be achieved through the application of external stimuli. In order to explore such an approach, elastomeric, nanoengineered, polymer photonic crystal structures have been fabricated on a large scale, through a method of shear induced self-assembly of 200nm monodisperse, polymer spheres with a core-shell structure. Determination of the assembly geometry through light diffraction experiments reveals a highly symmetric structure of close-packed, core-shell particles, with its orientation governed by the directionality imposed by the fabrication procedure. In these tuneable photonic crystals, application of external strain at directions of different crystallographic symmetry, accompanied by synchronised optomechanical measurements, reveals strong anisotropic optomechanical properties. It is shown that mechanical properties are primarily dominated by the viscoelastic nature of the shell material, while the strain-induced symmetry breaking reveals previously forbidden resonant peaks. Experiments involving uniaxial extension at principal and non-principal directions verify the underlying symmetry of the crystal lattice and consistently reproduce the anisotropic optical properties, providing information regarding the dual microstructure that controls the optomechanical response of these systems. Simulations based on a model of close-packed hard spheres predict the appearance of secondary resonances and suggest a structural transition from an fcc to a lower symmetry monoclinic crystal lattice. A more elaborate micromechanical model does not verify this transition but predicts the strain dependence of dominant spectroscopic peaks. Experiments involving different crosslinking densities reveal individual contributions from the elements comprising the material's dual microstructure. The inherently low refractive index contrast featured by these polymeric systems forbids the development of full photonic band gaps but symmetry based principles can be applicable to other structures with similar topological restrictions. Results provide a possible route for fabrication of active deformable nanostructures and aid our understanding of self-assembly in these complex systems, leading to optimised large-scale fabrication.
| Identifer | oai:union.ndltd.org:bl.uk/oai:ethos.bl.uk:600533 |
| Date | January 2014 |
| Creators | Kontogeorgos, Andreas |
| Publisher | University of Cambridge |
| Source Sets | Ethos UK |
| Detected Language | English |
| Type | Electronic Thesis or Dissertation |
| Source | https://www.repository.cam.ac.uk/handle/1810/245235 |
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