08 Fakultät Mathematik und Physik
Permanent URI for this collectionhttps://elib.uni-stuttgart.de/handle/11682/9
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Item Open Access Complex 2D & 3D plasmonic nanostructures : Fano resonances, chirality, and nonlinearities(2013) Hentschel, Mario; Giessen, Harald (Prof. Dr.)This thesis covers two topics of the still emergent field of plasmonics. On the one hand we make use of the interaction of particle plasmon resonances to create 2D as well as 3D complex plasmonic structures which show radically different optical properties than the individual building blocks do. On the other hand we utilize the strongly enhanced local electric field associated with plasmonic nanostructures for nonlinear optical processes. In particular, we study the formation of Fano resonances in complex nanoparticles arrangements. So-called plasmonic oligomers, that are highly symmetric arrangements of metallic nanoparticles, are discussed in detail. These clusters support dark modes which lead to pronounced scattering minima in their otherwise broad dipolar scatting peaks. We demonstrate the amazing tunability of these clusters and the formation of higher order dark modes. Moreover, we discuss the plasmonic analogue of electromagnetically induced transparency (EIT) in 2D as well as 3D arrangements of metallic nano-bars. We show that such 3D particle groupings are capable of encoding their 3D arrangement in well pronounced and unique optical spectra. We thus envision that our structure can serve as a three-dimensional plasmon ruler enabling the optically determination of three-dimensional arrangements on the nanoscale. Taking the concept of plasmonic EIT one step further, we demonstrate that the destructive interference between normal plasmonic modes, which leads to plasmonic EIT and decreased absorbance in the structure, can be switch to constructive interference and thus enhanced absorbance. It can be argued that this phenomenon is the plasmonic analogue of electromagnetically induced absorbance (EIA). What is more, we discuss the formation of optical chirality in 3D arrangements of metallic nanoparticles which vastly outperform any naturally occurring chiral substances in the strength of their interaction with an external light field. We deduce the prerequisites for this strong response and demonstrate that only configurational chirality, that is a handed arrangement of equally sized particles, leads to a strong plasmonic chiral optical response. Compositional chirality, that is the use of different sized particles in an unhanded arrangement, is not favourable. This finding is in contrast to chemistry and molecular physics where a so-called chiral center, a carbon atom dressed with four different ligands, is the archetype chiral building block. Moreover, we show that it is possible to optically deduce the spatial arrangements of individual particles in these structures, as chirality is an inherently 3D property. Furthermore, we will demonstrate the formation of a strong and broadband chiral optical response upon the formation of charge transfer modes, that is, due to ohmic contact of the clusters constituents. Finally, we demonstrate the plasmonic analogue of diastereomers, structures possessing several chiral centers. We thus construct plasmonic composite structures consisting of two different handed sub-units. We show that the optical response, in striking contrast to their molecular counterparts, can be described in terms of fundamental building blocks. The chiral optical response of such complex structures can thus be traced back to the optical properties of the constituting elements. Finally, we investiagte nonlinear optical processes in plasmonic and plasmonic-dielectric-hybrid systems. In particular, we investigate third harmonic generation from dimer nanoantennas and show that the nonlinear optical response, in contrast to common belief, is not governed by gap nonlinearities but fully described by the linear optical properties of the antenna. A simple nonlinear harmonic oscillator model is shown to reproduce all experimental features. Moreover, we will discuss the selective filling of bowtie nanoantennas with the chi2 active material LiNbO3 and the nonlinear optical response of this hybrid system. As an outlook we discuss the role of symmetries in nonlinear optics and the perceived implications for nonlinear plasmon optics.