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while polyvinylamine is an example of a weak polybase: (-CH2-CH-)n NH2 A second type of poly ion assumes stable, specific conformation. This group includes many natural poly electrolytes. For example, the side chains of proteins have a large number of acidic and basic ionizable groups. The resultant sign and amount of charge of the polyion depends on the pH (the species being a polyampholyte). The tertiary structure of the globular protein is so stable that it is not denatured even at a high value of the overall charge. Another example is the native form of deoxyribonucleic acid, whose double helix is quite stable in solution; the polyion acts in solution as a rigid rod. The difference in behaviour between polyion with a fixed shape and that of low-molecular-weight ions in solution depends only on their size and their overall charge. The behaviour in solution of the first type of polyions compared with that of uncharged molecules is more involved in that the coil expansion is affected not only by the solvent but also by the electric field formed by the polyion itself, by the counterions and by the ions of other low-molecularweight electrolytes, if present in the solution. Infinite charge dilution cannot be achieved by diluting the poly electrolyte solution, as a local high-intensity

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interactions of the chiral molecule with its nematogenic neighbors, the anisotropy of the nematic host phase, and on the order parameter (Goossens, 1971). HTP is related to the helical pitch by the following equation (De Gennes and Prost, 1993): HTP 1 pc 10:2

6

Fig. 1.15 A schematic representation of a polyacid solution including polyanions , anions of an added low molecular electrolyte O and positive counterions #

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where c is the concentration of the dopant. Thus, higher HTP values require less chiral dopant to yield the same l value. In addition, it is reported that HTP of the chiral dopants depends on their structures, and the chiral dopants with LC-like structure possess relatively higher HTP. Generally, anisotropic molecular shapes, such as rod shape, are required for liquid crystallinity and the appearance of LC phases (Demus, 1998; De Gennes and Prost, 1993). Therefore, if the shapes of molecules in LCs can be changed photochemically, LC properties including helical pitch length can be switched photochemically. Many studies have been done on photocontrolling of helical strcuture of Ch LCs through photoisomerization of various types of photochromic compounds, with/without chiral groups in molecules, such as azobenzenes (Bobrovsky and Shibaev, 2005; Kumaresan et al., 2005; Pieraccini et al., 2004; van Delden et al., 2004; Mallia and Tamaoki, 2003; Tamaoki et al., 2003; Bobrovsky and Shibaev, 2002; Ruslim and Ichimura, 2002; Moriyama and Tamaoki, 2001; Ruslim and Ichimura, 2001; Lee et al., 2000; Ruslim and Ichimura, 2000, Tamaoki et al., 2000;

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electric field remains inside the macroion, attracting a corresponding number of counterions (see the scheme in Fig. 1.15). Thus, the concept of the ionic strength of the solution lacks sense as an infinitely dilute solution of a polyelectrolyte does not behave ideally at any conditions and cannot be considered to be in the standard state. On the other hand, mutual repulsion of charges on the chain can lead to considerable chain expansion, which could not be achieved by transfer of the uncharged macromolecules from a 'bad' to a 'good' solvent. The shape of any macromolecule with a flexible chain, both uncharged and charged, i.e. the degree of expanding or rolling-up the random coil, is characterized by the parameter h, corresponding to the distance between the ends of the original chain from which the coil is formed. The probability that the ends will lie at a distance h is characterized by the probability density w(h) derived in textbooks on macromolecular chemistry by statistical methods on the basis of various models with various simplifying assumptions. In the resultant equations the number of basic segments in the macromolecule, Z, and their length, b> is taken into account and the actual system is described more or less accurately (and the equations are more or less complex) depending on the accuracy of the model employed. For polyelectrolytes, w(h) consists of the a priori probability wo(h), corresponding to the uncharged macromolecule, and the Boltzmann factor,

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Sackmann, 1971) , stilbenes (Haas et al., 1974), menthones (Van de Witte et al., 1999, 1998; Brehmer et al., 1998), diarylethenes (Yamaguchi et al., 2001; Denekamp and Feringa, 1998), overcrowded alkenes (Eelkema et al., 2006; van Delden et al., 2003; Feringa et al., 1995), and ugides (Sagisaka and Yokoyama, 2000). When the photochromic compounds with chiral groups are dissolved in a nematic LC, phototuning of the induced helical structure can be easily achieved by the use of suitable light, leading to a difference in HTP between photoisomers through photochemical change in their molecular shapes. Azobenzene molecules undergo reversible trans cis photoisomerization by irradiation of light with appropriate wavelength (Ross and Blank, 1971), and when a chiral azobenzene molecule is doped in Ch LCs, its HTP can be changed by reversible photoisomerization. Thus, according to Eq. 10.2, the helical pitch can be controlled through reversible photoisomerization. Azobenzene systems represent very attractive phototriggers in Ch LCs, thanks to their resistance to photofatigue, the simplicity of the molecules, and the ease of modi cation of their molecular structures. This chapter rst describes helical twisting ability of chiral azobenzene compounds by focusing the structural effects on HTP as well as photochemical change in HTP, and then phototuning of helical structures of Ch LCs through the trans cis photoisomerization of the chiral azobenzene compounds for applications to optical devices.

77 containing the excess electrostatic Gibbs energy AGf,(/*): w(h) dh = wo(h) exp ( ~ A ^ l ( / l ) ) d* (1.5.18)

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