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1998; Kim et al, 1997; Rochon et al, 1995) and single-beam surface deformations (Bian et al, 1998) convincingly showed that the light and surface relief are 1801 out of phase In other words, light intensity maxima correspond to valleys in the surface relief In effect, material is moved out of the light and into the dark regions This rule appears to hold in the majority of cases, yet in a number of systems the phase relationship seems to be exactly inverted, with mass transport into illuminated regions Speci cally, in certain liquid crystalline (LC) systems, the phase behavior is inverted (Helgert et al, 2001; Bublitz et al, 2000; Holme et al, 1999) In one study, an amorphous material exhibited the usual phase behavior, and a thin lm of this polymer oating on water expanded in the direction of the light polarization.

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A similar LC azopolymer exhibited inverted phase behavior in SRG experiments, and contracted in the direction of polarized illumination as a oating lm The tempting conclusion is that amorphous and polymeric systems exhibit opposite photomechanical response, which translates into opposite phase behavior in grating inscription A possibly relevant experiment showed that for LC systems, the cis chromophores may become preferentially oriented along the light polarization direction, instead of being perpendicular to it (Hore et al, 2003) It should be pointed out, however, that some LC systems exhibit the usual phase relationship (Zettsu et al, 2003), and in one LC system, modi cation of a single ring substituent led to opposite phase behavior (Helgert et al, 2001) Adding to the complexity of the phase relationship, it was observed that at high irradiation power (W300 W/cm2), the behavior was inverted in amorphous systems (Bian et al, 1999).

Single-beam experiments at high power showed a central peak instead of a depression By exposing a sample to a gradient two-beam intersection, a lm was inscribed with a continuum of laser intensitites An inphase grating was found in the high power region, and a conventional out-ofphase SRG was found in the low power region The intermediate region clearly showed interdigitation of the peaks from the two regimes, resembling a doubling of grating period observed by others These double-period gratings can be formed in a number of amorphous systems, using the polarization combinations of ( p, p) or (+451, 451), with indications that even the (s, s) and ( p, s) combinations function to a certain extent (Lagugne-Labarthet et al, 2004; Labarthet et al, 2001, 2000; Naydenova et al, 1998a) Observations of a double-frequency orientational grating underneath a normal SRG have also been reported (Schaller et al.

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, 2003) The double-period SRGs were attributed to interference between the diffracted beams from the primary grating, which gives rise to a light modulation, with double the initial frequency, in the material Whether these double-period gratings are related to the inverted structures observed in high intensity experiments and some LC systems is an open question It is interesting to note that some of the amorphous polymers that exhibit double-frequency behavior have accessible LC phases at a higher temperature These phase behavior results strongly suggest that there are (at least) two mechanisms at play during surface patterning One dominates at low intensity in amorphous systems, whereas another appears to dominate at higher intensity and in LC systems From an applied standpoint,.

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