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393 5.10.3 Homogeneous photoredox reactions and photogalvanic effects The photogalvanic effects are initiated by a homogeneous photoredox reaction of an electrolyte redox system with a suitable photoexcited organic or organometallic substance (dye), S. The photon absorption produces a short-lived, electronically excited dye molecule, S*:
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whose structure and physicochemical properties are different. The conversion of 5* back to 5 proceeds by various radiative and non-radiative relaxation processes, which are characterized by a pseudo-first-order rate constant, kb. Its reciprocal value defines the lifetime of the excited state, r0: ro=l/kb (5.10.2)
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to the grating direction could be attributed to photoaggregation of the azo dye molecules or buckling of the elastomeric surface. Indeed all of these otherwise contradictory results can be reconciled by considering a more general photomechanical explanation, where both photoexpansion (for materials below a crossover mobility temperature; i.e., amorphous) and photocontraction (for materials above a mobility threshold; i.e., liquid crystal samples) both occur (Yager and Barrett, 2006b). Further investigations into reconciling this model with the polarization dependence of inscription are in order, where presumably photoorientation will play a key role.
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(the fraction of the S* molecules, deactivated during the time r 0 , equals 1 e~l 63%). Only excitations of electrons from the highest occupied molecular orbital (HOMO) to the lowest unoccupied molecular orbital (LUMO), which produce reasonably long-lived S* molecules are practically important. This is schematically depicted in Fig. 5.57. Most of the ground-state molecules contain all the electrons paired. (The 0 2 molecule is an important exception to this rule.) The excited molecule may occur in two states, either with none or two unpaired electrons; these states are called excited singlet, 5X, or excited triplet, Tx. The latter state is, according to the Pauli rule, energetically favoured and its lifetime is higher by orders of magnitude, since the reactions with singlet molecules as well as radiative relaxation (phosphorescence) are spin-forbidden. The photoexcited S*{TX) molecule may have a sufficiently long lifetime to diffuse some distance in the electrolyte solution and to take part in a
The single-step, rapid, and reversible all-optical surface patterning effect discovered in a wide variety of azobenzene systems has, of course, been suggested as the basis for numerous applications Azobenzene is versatile, amenable to incorporation in a wide variety of materials The mass patterning is reversible, which is often advantageous However, one may use a system where cross-linking enables permanent xation of the surface patterns (Zettsu et al, 2001) Many proposed applications are optical and t well with azobenzene s already extensive list of optical capabilities The gratings have been demonstrated as optical polarizers (Tripathy et al, 2000), angular or wavelength lters (Stockermans and Rochon, 1999; Rochon et al, 1997), and couplers for optical devices (Paterson et al, 1996) They have also been suggested as photonic band gap materials (Nagata et al.
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, 2001), and have been used to create lasers where emission wavelength is tunable via grating pitch (Rocha et al, 2001; Dumarcher et al, 2000) The process has, of course, been suggested as an optical data storage mechanism (Egami et al, 2000) The high speed and single-step holographic recording has been suggested to enable instant holography (Ramanujam et al, 1999), with obvious applications for industry or end consumers Since the hologram is topographical, it can easily be used as a master to create replicas via molding The surface patterning also allows multiple holograms to be superimposed, if desired A novel suggestion is to use the patterning for rapid prototyping of optical elements (Neumann et al, 1999) Optical elements could be generated or modi ed quickly and during device operation They could thereafter be replaced with permanent components, if required.
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