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Crystal field effects, nonlinear optical

Recently, many researchers have studied fine particles or microcrystals to clarify the intermediate state between bulk crystals and isolated atoms and molecules (12-16). From these studies in the field of nonlinear optics, Hanamura predicted excitonic and surface-state enhancements of third-order optical nonlinearity in microcrystals because of quantum confinement effects, which is one of several size effects theoretically established by Ekimov et al. and Brus (17-19). Following these theories, enhancements of have been reported in semiconductor-microcrystallite-doped glasses and polymers (20,21). Organic microcrystals, however, have attracted very little attention so far (22,23) owing to the difficulties of preparing them. [Pg.184]

Optical harmonic generation is one of the earliest and most developed area in the field of nonlinear optics. Not surprisingly, investigations of nonlinear optical effects in liquid crystals started also with the study of harmonic generation. The aim of the first studies was to observe second harmonic generation (SHG) in cholesteric liquid crystals. [Pg.11]

In the present volume we discuss a relatively new and rapidly developing branch of the field, namely nonlinear optical effects in liquid crystals. Optical studies have always played a significant role in liquid crystal science. Research of optical nonlinearities in liquid crystals began at the end of the sixties. Since then it became a powerful tool in the investigation of symmetry properties, interfacial phenomena or dynamic behaviour. Furthermore, several new aspects of nonlinear processes were demonstrated and studied extensively in liquid crystals. The subject covered in this book is therefore of importance both for liquid crystal research and for nonlinear optics itself. [Pg.240]

Liquid crystal polymers are also used in electrooptic displays. Side-chain polymers are quite suitable for this purpose, but usually involve much larger elastic and viscous constants, which slow the response of the device (33). The chiral smectic C phase is perhaps best suited for a polymer field effect device. The abiHty to attach dichroic or fluorescent dyes as a proportion of the side groups opens the door to appHcations not easily achieved with low molecular weight Hquid crystals. Polymers with smectic phases have also been used to create laser writable devices (30). The laser can address areas a few micrometers wide, changing a clear state to a strong scattering state or vice versa. Future uses of Hquid crystal polymers may include data storage devices. Polymers with nonlinear optical properties may also become important for device appHcations. [Pg.202]

Two of the most important nonlinear optical (NLO) processess, electro-optic switching and second harmonic generation, are second order effects. As such, they occur in materials consisting of noncentrosymmetrically arranged molecular subunits whose polarizability contains a second order dependence on electric fields. Excluding the special cases of noncentrosymmetric but nonpolar crystals, which would be nearly impossible to design from first principles, the rational fabrication of an optimal material would result from the simultaneous maximization of the molecular second order coefficients (first hyperpolarizabilities, p) and the polar order parameters of the assembly of subunits. (1)... [Pg.270]

The EO effect is a second-order nonlinear optical (NLO) effect. Only non-centrosymmetrical materials exhibit second-order NLO effects. This non-centrosymmetry is a condition, both at the macroscopic level of the bulk arrangement of the material and at the microscopic level of the individual molecule. All electro-optic modulators that are presently used by telecom operators are ferro-electric inorganic crystals. The optical nonlinearity in these materials is to a large fraction caused by the nuclear displacement in the applied electric field, and to a smaller fraction by the movement of the electrons. This limits the bandwidth of the modulator. The nonlinear response of organic materials is purely electronic and, therefore, inherently faster. [Pg.380]

The Pockel s effect [3] refers to an electro-optical process wherein the application of large electric fields onto crystals lacking a center of symmetry can lead to nonlinear polarization effects and optical rotation. Pockel cells can be used in place of photoelastic modulators and can achieve very high modulation frequencies but often have the undesirable property of a nonzero birefringence in the absence of an applied field. [Pg.163]

In tune with the above introductory remarks, we have arranged this review in the following way Section II deals with the oriented gas model that employs simple local field factors to relate the microscopic to the macroscopic nonlinear optical responses. The supermolecule and cluster methods are presented in Section III as a means of incorporating the various types of specific interactions between the entities forming the crystals. The field-induced and permanent mutual (hyper)polarization of the different entities then account for the differences between the macroscopic and local fields as well as for part of the effects of the surroundings. Other methods for their inclusion into the nonlinear susceptibility calculations are reviewed in Section IV. In Section V, the specifics of successive generations of crystal orbital approaches for determining the nonlinear responses of periodic infinite systems are presented. Finally,... [Pg.43]

The oriented gas model was first employed by Chemla et al. [4] to extract molecular second-order nonlinear optical (NLO) properties from crystal data and was based on earlier work by Bloembergen [5]. In this model, molecular hyperpolarizabilities are assumed to be additive and the macroscopic crystal susceptibilities are obtained by performing a tensor sum of the microscopic hyperpolarizabilities of the molecules that constitute the unit cell. The effects of the surroundings are approximated by using simple local field factors. The second-order nonlinear response, for example, is given by... [Pg.44]

In my view, this book contains the most in-depth and broad-based discussion of molecular nonlinear materials yet available. While it does not in itself discuss all the issues (there is relatively little on molecular crystals or on local-field effects), the combination of theoretical and experimental presentations makes the book of unique value to any investigators in the general of molecular nonlinear optics. [Pg.692]

The theory of nonlinear optical processes in crystals is based on the phenomenological Maxwell equations, supplemented by nonlinear material equations. The latter connect the electric induction vector D(r,t) with the electric field vector E(r, t). In general, the relations are both nonlocal and nonlinear. The property of nonlocality leads to the so-called spatial dispersion of the dielectric tensor. The presence of nonlinearity leads to the interaction between normal electromagnetic waves in crystals, i.e. makes conditions for the appearance of nonlinear optical effects. [Pg.229]


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