Nonlinear optics in complex, chiral, and 3D plasmonic nanostructures

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In this proposal, we are going to study the nonlinear optical response of complex plasmonic nanostructures upon exposure to ultrafast laser pulses. Our goal is to understand the nonlinear optical tensor for second- and third-harmonic generation in an ab-initio fashion. In particular, we are going to utilize complex plasmonic structures such as hybrid nanoantennas, 2- and 3-dimensional complex oligomers, and 3-dimensional chiral plasmonic metamaterials as nonlinear media. Furthermore, we will utilize hybrid structures, where the complex plasmonic nanostructures are being combined with dielectric nanostructures which exhibit Chi(2) or Chi(3) nonlinearities themselves. We are going to utilize time-integrated as well as time-resolved spectroscopy, and we will study the effects for different wavelengths and polarizations, as well as their angle dependence. Our work should lead not only to a fundamental understanding of the nonlinear optical mechanisms that can be enhanced largely by tailoring appropriate plasmonic nanostructures, but also to novel applications, such as plasmonically enhanced mid-IR and THz generation as well as nonlinear plasmonic sensing.