Electronic Thesis and Dissertation Repository

Degree

Doctor of Philosophy

Program

Physics

Supervisor

Dr. François Lagugné-Labarthet

Abstract

The understanding of optical properties of surfaces and interfaces are critical for the development of new technologies ranging from photonics to molecular electronics. Knowing for example the orientation of molecules functionalized onto a surface yields valuable information about the macroscopic properties of the resulting surface. The optical properties can be tuned using various strategies such as molecular functionalization or patterning of meta-structures that ultimately interact with light in a rational way. Advanced optical and spectroscopy methods allowing one to probe such surfaces are therefore key to correlate properties and surface functionalization.

In this thesis, multiple approaches have been taken to understand the optical response of anisotropic interfaces. First, polarization-modulation infrared linear dichroism is used to characterize thin films of azobenzene-containing glasses and follow the dynamic of their orientation. Because of the high charge-transfer of these molecules their nonlinear properties are also investigated using second harmonic generation microscopy under microscopy conditions. The coupling of nonlinear active molecules with metallic nanostructures is also investigated using SHG to evaluate the plasmonic enhancements from the nanostructures alone or functionalized with molecules with high hyperpolarizability.

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