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Fig. 1.8 Dependence of the mean activity coefficient y >c of NaCl on the square root of molar concentration c at 25 C. Circles are experimental points. Curve 1 was calculated according to the Debye-Hiickel limiting law (1.3.25), curve 2 according to the approximation aB = 1 (Eq. 1.3.32); curve 3 according to the Debye-Hiickel equation (1.3.31), fl = 325nm; curve 4 according to the BatesGuggenheim approximation (1.3.33); curve 5 according to the Bates-Guggenheim approximation + linear term 0.1 C; curve 6 according to Eq. (1.3.38) for a=0.4nm, C = 0.055 dm 5 -mor 1 ionic atmosphere is then given by the expressions -1 (1.3.26)

inscription. A further elaboration took into account induced anisotropy in the lm and associated anisotropic polymer lm deformation (expansion or contraction in the electric eld direction) (Bublitz et al., 2001). The assumption of an anisotropic deformation is very much consistent with experimental observations (Bublitz et al., 2000). Such an analysis, remarkably, was able to reproduce most of the polarization dependence, predict phase-inverted behavior at high power, and even demonstrated double-period (interdigitated) gratings. A nonlinear stressrelaxation analysis could account for the nonlinear response during intermittent (pulselike) exposure (Saphiannikova et al., 2004b). Finite-element linear viscoelastic modeling enabled the inclusion of nite compressibility (Saphiannikova et al., 2004a). This allowed the nonlinear intermittent-exposure results, and, critically, the formation of DGs, to be correctly predicted. This analysis also demonstrated, as expected, that surface tension acts as a restoring force that limits grating amplitude (which explains the eventual saturation). Finally, the kinetics of grating formation (and erasure) have been captured in a lattice Monte Carlo simulation that takes into account isomerization kinetics and angular redistribution of chromophores (Mitus et al., 2004; Pawlik et al., 2004, 2003). Thus, the nonlinear viscoelastic ow and deformation (compression and expansion) of polymer material appear to be well understood. What remains to be fully elucidated is the origin of the force inside the material. More speci cally, the connection between the azobenzene isomerization and the apparent force must be explained.

(1.3.27)

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Models involving thermal effects were proposed when SRG formation was rst observed. Although simple and appealing, a purely thermal mechanism would not account for the polarization dependence that is observed experimentally. The grating formation proceeds at remarkably low laser power, thus thermal mechanisms appear untenable. A more detailed modeling analysis (Yager and Barrett, 2004) showed that the temperature gradient induced in a sample under typical SRG formation conditions was on the order of 10 4 K. This thermal gradient is much too small for any appreciable spatial variation of material properties. The net temperature rise in the sample was found to be on the order of 5 K, which again suggests that thermal effects (such as temperature-induced material softening) are negligible. However, high intensity experiments have shown the formation of gratings that could not be subsequently thermally erased (Bian et al., 1999). It is likely that in these cases a destructive thermal mechanism plays a role. In nanosecond-pulsed experiments, gratings can be formed (Si et al., 2002; Leopold et al., 2000; Ramanujam et al., 1999; Schmitt et al., 1997). However, these gratings are because of irreversible ablation of the sample surface, a phenomenon well established in high power laser physics. Moreover, the formation of gratings at these energies does not require azobenzene: any absorbing chromophore will do (Baldus et al., 2001). Computer modeling con rms temperature rises on the order of B8000 K for nanosecond pulses (Yager and Barrett, 2004), clearly an entirely

a (nm)

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different regime from the facile room temperature patterning unique to azo chromophores. Although thermal effects should be considered for a complete understanding of SRG formation (especially the phase-inverted structures observed at higher power), they appear to be negligible for typical irradiation conditions at modest laser power.