Crystal field effects, nonlinear optical properties

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. 

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. 

Certain glass-ceramic materials also exhibit potentially useful electro-optic effects. These include glasses with microcrystaUites of Cd-sulfoselenides, which show a strong nonlinear response to an electric field (9), as well as glass-ceramics based on ferroelectric perovskite crystals such as niobates, titanates, or zkconates (10—12). Such crystals permit electric control of scattering and other optical properties. 

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. 

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... 

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. 

Liquid crystals are generally characterized by the strong correlation between molecules, which respond cooperatively to external perturbations. That strong molecular reorientation (or director reorientation) can be easily induced by a static electric or magnetic field is a well-known phenomenon. The same effect induced by optical fields was, however, only studied recently. " Unusually large nonlinear optical effects based on the optical-field-induced molecular reorientation have been observed in nematic liquid-crystal films under the illumination of one or more cw laser beams. In these cases, both the static and dynamical properties of this field-induced molecular motion are found to obey the Ericksen-Leslie continuum theory, which describe the collective molecular reorientation by the rotation of a director (average molecular orientation). 

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