Abstract
SECOND-harmonic generation (SHG)—the frequency doubling of light—requires materials with a non-centrosymmetric structure that gives rise to a large second-order nonlinear optical susceptibility. For molecular materials, it is widely assumed that the molecular structure, as well as the packing arrangement, must also be non-centrosymmetric, unless a magnetic dipole1–3 or an electric quadrupole4 contributes to the bulk susceptibility. Consequently, most studies have focused on dipolar molecular systems in which the optical nonlinearities arise from intramolecular charge transfer5–8. But the criteria for SHG may also be satisfied by centrosymmetric molecules if they aggregate in a non-centrosymmetric manner and there is a contribution to the bulk susceptibility from intermolecular charge transfer. Here we report the nonlinear optical properties of a series of centrosymmetric dyes based on a squaraine template, which we ascribe to such an effect. Monolayer films of these molecules deposited by the Langmuir–Blodgett (LB) technique show surprisingly large SHG, which compares favourably with the highest hitherto reported for LB monolayers of non-centrosymmetric molecules.
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Ashwell, G., Jefferies, G., Hamilton, D. et al. Strong second-harmonic generation from centrosymmetric dyes. Nature 375, 385–388 (1995). https://doi.org/10.1038/375385a0
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DOI: https://doi.org/10.1038/375385a0
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