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A series of ferrocenyl substituted pyrazaboles were prepared, which have an electron-withdrawing pyrazabole moiety as the central core, with a D–π–A–π–D structural motif (D = donor, A = acceptor) and containing a variety of π bridges. A crystallographic study reveals that the pyrazabole central core was observed in planar geometry. Strong two-photon absorption in the visible region and three-photon absorption in the near IR region were observed in the ferrocenyl substituted pyrazaboles. It was observed that the 2PA absorption cross-section increases with the conjugation length.
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