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Molecules 2016, 21(5), 647; doi:10.3390/molecules21050647

Broadband Two-Photon Absorption Characteristics of Highly Photostable Fluorenyl-Dicyanoethylenylated [60]Fullerene Dyads

1
Department of Chemistry, Institute of Nanoscience and Engineering Technology, University of Massachusetts Lowell, Lowell, MA 01854, USA
2
Department of Physics, National University of Singapore, Singapore 117542, Singapore
3
Functional Materials Division, AFRL/RXA, Air Force Research Laboratory, Wright-Patterson Air Force Base, Dayton, OH 45433, USA
*
Authors to whom correspondence should be addressed.
Academic Editor: Derek J. McPhee
Received: 27 March 2016 / Revised: 27 April 2016 / Accepted: 6 May 2016 / Published: 14 May 2016
(This article belongs to the Special Issue Fullerene and the Related Curved-pi Materials Chemistry)
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Abstract

We synthesized four C60-(light-harvesting antenna) dyads C60 (>CPAF-Cn) (n = 4, 9, 12, or 18) 1-Cn for the investigation of their broadband nonlinear absorption effect. Since we have previously demonstrated their high function as two-photon absorption (2PA) materials at 1000 nm, a different 2PA wavelength of 780 nm was applied in the study. The combined data taken at two different wavelength ranges substantiated the broadband characteristics of 1-Cn. We proposed that the observed broadband absorptions may be attributed by a partial π-conjugation between the C60 > cage and CPAF-Cn moieties, via endinitrile tautomeric resonance, giving a resonance state with enhanced molecular conjugation. This transient state could increase its 2PA and excited-state absorption at 800 nm. In addition, a trend of concentration-dependent 2PA cross-section (σ2 ) and excited-state absorption magnitude was detected showing a higher σ value at a lower concentration that was correlated to increasing molecular separation with less aggregation for dyads C60(>CPAF-C18) and C60(>CPAF-C9), as better 2PA and excited-state absorbers. View Full-Text
Keywords: C60-(light-harvesting antenna) nanostructures; Z-scan measurements; ultrafast two-photon absorption; nonlinear absorption C60-(light-harvesting antenna) nanostructures; Z-scan measurements; ultrafast two-photon absorption; nonlinear absorption
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This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. (CC BY 4.0).

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Jeon, S.; Wang, M.; Ji, W.; Tan, L.-S.; Cooper, T.; Chiang, L.Y. Broadband Two-Photon Absorption Characteristics of Highly Photostable Fluorenyl-Dicyanoethylenylated [60]Fullerene Dyads. Molecules 2016, 21, 647.

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