For supramolecular compounds with donor and acceptor fragments, coupled with each other by the <$E pi>-conjugated methyn chain, it was ascertained an influence of Cl and Br atoms on the <$E pi>-conjugation and charge transfer in them in molecular and aggregate states. Compound, which contains Br atom, crystallizes into a noncentrosymmetric polar structure and under infrared (1064 nm) laser excitation it is observed the second harmonic generation and intense up-conversion photoluminescence in the visible spectral region. For compounds containing Cl atom, when passing into a crystalline state, only up-conversion photoluminescence is observed, which can be considered as two-photon excited. Possible mechanisms of intramolecular charge transfer and collective interactions in investigated molecular structures under one- and two-photon excitation are considered.

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