Macroscopic Motion in Java

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1.2.5. Macroscopic Motion
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It is interesting to study whether the azobenzene molecular conformational rearrangements can result in changes to bulk phenomena, or even to macroscopic motion. The rst consideration is whether the material expands to an appreciable extent. In monolayers, it is well established that the larger molecular size of the cis isomer leads to a corresponding lateral expansion (Higuchi et al., 1995b), which can modify other bulk properties. For instance, this allows photomodulation of a monolayer s water contact angle (Siewierski et al., 1996) or surface potential (Stiller et al., 1999). Using uorinated azo polymer, good photocontrol (Feng et al., 2001) and photopatterning (Moller et al., 1998) of wettability has been demonstrated. A monolayer of azo-modi ed calixarene, when irradiated with a light gradient, produced a gradient in surface energy suf cient to move a macroscopic oil droplet (Ichimura et al., 2000), suggesting possible applications in micro uidics. Modest photoinduced contact angle changes for thin polymer lms have also been reported (Sarkar et al., 2001). Recently an azobenzene copolymer assembled into polyelectrolyte multilayer showed a modest 21 change in contact angle with UV light irradiation. However, when the same copolymer was assembled onto a patterned substrate, the change in contact angle upon irradiation was enhanced to 701 (Jiang et al., 2005). It is well established that
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surface roughness plays a role in contact angle and many systems can be optimized to give rise to a large change in surface properties. In layered inorganic systems with intercalated azobenzenes, reversible photochanges in the basal spacing (on the order of 4%) can be achieved (Fujita et al., 1998, 2001). In polymer lms, there is some evidence that the lm thickness increases, as measured by ellipsometry (Shi et al., 1991b) (the refractive index certainly changes [Ivanov et al., 1995], but this is not an unambiguous demonstration of expansion contraction). Experiments that show that external applied pressure tends to hinder photoisomerization (Kleideiter et al., 2000) are related. Photocontraction for semicrystalline main-chain azos has been measured (Eisenbach, 1980b; Agolini and Gay, 1970). This photomechanical response presumably occurs because of the shortening of the polymer chains upon trans-cis conversion. However, photoexpansion would seem to be contradicted by positron lifetime experiments that suggest no change in microscopic free volume cavity size during irradiation (Algers et al., 2004). More conclusive experiments are in order. The most convincing demonstration of macroscopic motion due to azo isomerization is the mechanical bending and unbending of a free-standing polymer lm (Ikeda et al., 2003; Yu et al., 2003). The macroscopic bending direction may be selected either with polarized light or by aligning the chromophores with rubbing. Bending occurs in these relatively thick lms because the free surface (which absorbs light) contracts, whereas the interior of the lm (which is not irradiated owing to the strong absorption of the upper part of the lm) does not contract. Because the direction of bending can be controlled with polarized light, the materials enable full directional photomechanical control (Yu et al., 2005). This photomechanical deformation has also been used to drive macroscopic motion of a oating lm (Camacho-Lopez et al., 2004). That these materials contract (rather than expand) appears again to be related to the main-chain azo groups and may also be related to the LC nature of the cross-linked gels. For a thin lm oating on a water surface, a contraction in the direction of polarized light was seen for LC materials, whereas an expansion was seen for amorphous materials (Bublitz et al., 2000). A related ampli cation of azo motion to macroscopic motion is the photoinduced bending of a microcantilever coated with an azobenzene monolayer (Ji et al., 2004). One can also invert the coupling of mechanical and optical effects: by stretching an elastomeric azo lm containing a grating, one can affect its wavelength-selection properties and orient chromophores (Bai and Zhao, 2001).
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