Advanced Materials

Large third-order nonlinear optical response from molecules with effective multidirectional charge-transfer transitions: New design of third-order nonlinear chromophores

Authors

  • Daniel R. Greve,

    1. CISMI, Department of Chemistry Symbion, University of Copenhagen Fruebjergvej 3, DK-2100 Copenhagen (Denmark)
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  • Steen B. Schougaard,

    1. CISMI, Department of Chemistry Symbion, University of Copenhagen Fruebjergvej 3, DK-2100 Copenhagen (Denmark)
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  • Dr. Tommy Geisler,

    1. Institute of Physics, Aalborg University Pontoppidanstrxde 103 DK-9220 Aalborg Øst (Denmark)
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  • Dr. Jan C. Petersen,

    1. Danish Institute of Fundamental Metrology Bldg. 307, Anker Engelunds Vej 1, DK-2800 Lyngby (Denmark)
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  • Dr. Thomas Biørnholm

    Corresponding author
    1. CISMI, Department of Chemistry Symbion, University of Copenhagen Fruebjergvej 3, DK-2100 Copenhagen (Denmark)
    • CISMI, Department of Chemistry Symbion, University of Copenhagen Fruebjergvej 3, DK-2100 Copenhagen (Denmark)
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  • We thank Dr. Peter Sommer-Larsen for fruitful discussions and the EU HCM network “Novel third-order nonlinear optical materials” as well as the Danish Research Councils for financial support.

Abstract

Enhanced values of the second molecular hyperpolarizability, γ, are reported for molecules that undergo significant multidirectional charge redistributions between the ground and excited states, e.g., charge is displaced from the periphery to the center, or vice versa, upon excitation, in during large changes in electric moments higher than dipole moments. The γ-values are compared with those for polyene-like molecules having a similar number of π-electrons. It is demonstrated that the “periphery-to-center charge-transfer” design concept is fruitful and should lead to new molecules with high γ-values.

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