Blue and green Čerenkov-type second-harmonic generation in a polymeric Langmuir–Blodgett waveguide

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Christopher R. Brown

2,4-Bis[4-(dihexadecylamino)-2-hydroxyphenyl]squaraine is vertically oriented in the Langmuir–Blodgett film and the chromophore layer is separated from the glass substrate by the hydrophobic dihexadecylamino groups. The Langmuir–Blodgett monolayer exhibits moderately strong second-harmonic generation (SHG) with an effective susceptibility of c. 10 pm V-1 at 1064 nm and an intensity, relative to the mean SHG from films of the extensively studied hemicyanine dye (E)-4-[2-(4-dimethylaminophenyl)ethenyl]-N-docosylpyridinium bromide, of c. 0·3. The SHG cannot arise from the polarization of the dye by the underlying substrate because the conjugated donor-(acceptor)-donor moiety is separated by a 2 nm thick hydrophobic barrier. Instead, the non-linear optical behaviour is attributed to a non-centrosymmetric aggregate structure.


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