Orientation nonlinear optics

Because of the generality of the symmetry principle that underlies the nonlinear optical spectroscopy of surfaces and interfaces, the approach has found application to a remarkably wide range of material systems. These include not only the conventional case of solid surfaces in ultrahigh vacuum, but also gas/solid, liquid/solid, gas/liquid and liquid/liquid interfaces. The infonnation attainable from the measurements ranges from adsorbate coverage and orientation to interface vibrational and electronic spectroscopy to surface dynamics on the femtosecond time scale. 

Zhuang X, Miranda P B, Kim D and Shen Y R 1999 Mapping molecular orientation and conformation at interfaces by surface nonlinear optics Phys. Rev. B 59 12 632-40... 

Microscopy methods based on nonlinear optical phenomena that provide chemical information are a recent development. Infrared snm-frequency microscopy has been demonstrated for LB films of arachidic acid, allowing for surface-specific imaging of the lateral distribution of a selected vibrational mode, the asymmetric methyl stretch [60]. The method is sensitive to the snrface distribntion of the functional gronp as well as to lateral variations in the gronp environmental and conformation. Second-harmonic generation (SHG) microscopy has also been demonstrated for both spread monolayers and LB films of dye molecules [61,62]. The method images the molecular density and orientation field with optical resolution, and local qnantitative information can be extracted. 

Bauer, W. S. Yilmaz, S. Wirges, W. Gerhard Multhaupt, R., Optimized poling of nonlinear optical polymers based on dipole orientation and dipole relaxation studies, J. Appl. Phys. 1994,75,7211 7219... 

As mentioned in this section, the linear Stark effect measurement provides detailed information on noncentrosymmetric molecular orientation. This technique is very helpful for the advanced molecular design of noncentrosymmetric LB films for electro-optic and nonlinear optic applications. 

Third-order nonlinear optical properties of oriented poly(arylenevinylene) LB films... 

Aromatic poly(benzothiazole)s are thermally and thermooxidatively stable and have outstanding chemical resistance and third-order nonlinear optical susceptibility. Aromatic poly(benzothiazole)s can be spun into highly-oriented ultrahigh strength and ultrahigh modulus fibers. However, this type of polymer is insoluble in most organic solvents. Therefore, hexafluoroisopropylidene units are introduced in the polymer backbone to obtain soluble or processable aromatic poly(benzothiazole)s. 

Kajzar, F, Lee, K.-S. and Jen, A. K.-Y Polymeric Materials and their Orientation Techniques for Second-Order Nonlinear Optics. Vol. 161, pp. 1-85. 

Motivating the research is the need for systematic, quantitative information about how different surfaces and solvents affect the structure, orientation, and reactivity of adsorbed solutes. In particular, the question of how the anisotropy imposed by surfaces alters solvent-solute interactions from their bulk solution limit will be explored. Answers to this question promise to affect our understanding of broad classes of interfacial phenomena including electron transfer, molecular recognition, and macromolecular self assembly. By combining surface sensitive, nonlinear optical techniques with methods developed for bulk solution studies, experiments will examine how the interfacial environment experienced by a solute changes as a function of solvent properties and surface composition. 

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