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Two C 60 -(antenna) x analogous compounds having branched hybrid triad C 60 (&gt;DPAF-C 18 )(&gt;CPAF-C 2M ) and tetrad C 60 (&gt;DPAF-C 18 )(&gt;CPAF-C 2M ) 2 nanostructures were synthesized and characterized. The structural design was intended to facilitate the ultrafast fs intramolecular energy-transfer from photoexcited C 60 [&gt; 1 (DPAF)*-C 18 ](&gt;CPAF-C 2M ) 1or2 or C 60 (&gt;DPAF-C 18 )[&gt; 1 (CPAF)*-C 2M ] 1or2 to the C 60 &gt; cage moiety upon two-photon pumping at either 780 or 980 nm, respectively. The latter nanostructure showed approximately equal extinction coefficients of optical absorption over 400-550 nm that corresponds to near-IR two-photon based excitation wavelengths at 780-1100 nm for broadband nonlinear optical (NLO) applications. Aside from their enhanced two-photon absorption (2PA) activity at 780 nm, we also demonstrated ultrafast photo-responses at 980 nm showing 2PA cross-section ( σ  2 ) values of 995-1100 GM for the hybrid tetrad. These σ  2 values were correlated to the observed good efficiency in reducing fs light-transmittance down to 35% at the light intensity of 110 GW/cm 2 . Accordingly, 2PA characteristics of these nanostructures at multiple NIR wavelengths provided support for their suitability in uses as broadband NLO nanomaterials at 600-1100 nm that includes the 2PA ability of two antenna, DPAF (700-850 nm) and CPAF (850-1100 nm), and the fullerene cage at shorter wavelengths (600-700 nm).

Linear and Nonlinear Optical Properties of Photoresponsive [60]Fullerene Hybrid Triads and Tetrads with Dual NIR Two-Photon Absorption Characteristics