We present a multipolar tensor analysis of second-harmonic generation from arrays of noncentrosymmetric gold nanoparticles. In contrast to earlier results, where higher multipoles and symmetry-forbidden signals arising from sample defects play a significant role, the present results are completely dominated by symmetry-allowed electric-dipole tensor components. The result arises from significant improvement in sample quality, which suppresses the higher-multipole effects and enhances the overall response by an order of magnitude. The results are a prerequisite for metamaterials with controllable nonlinear properties.
We perform a detailed characterisation of the second-order nonlinear optical response of nanocomposites consisting of alternating layers of silver-decorated silica glass nanoparticles and pure silica glass. The samples are fabricated using aerosol techniques and electron-beam dielectric coating, resulting in a bulk-like material with symmetry-breaking induced by the porosity of the alternating layers. The second-order nonlinear response increases with the number of layers. Further, by determining the components of the second-order susceptibility tensor of the samples, we show that the structural properties of the samples are well maintained as the sample thickness is increased. Our results form an important baseline for any further optimization of these types of structures, which can be fabricated using very straightforward methods.
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