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Nonlinear optical properties of novel tunable, one dimensional molecular superlattice polymers (heteroarylene methines) containing alternating aromatic and quinoid segments

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Abstract

We have investigated the spectral dispersion of second molecular hyperpolarizability γ (−ω′; ω, −ω, ω) of three derivatives of heteroarylene methine by antiresonant ring interferometric nonlinear spectroscopic technique using femtosecond modelocked Ti:sapphire laser in the spectral range of 725–820 nm. The observed dispersion of γ has been explained in the framework of three-essential states model involving the ground state, a one-photon excited state and a two-photon excited state. The spectral response of the hyperpolarizability has been correlated with the electronic and chemical structures of the three derivatives of heteroarylene methine. The estimated γ values have been compared to the fundamental quantum mechanical limit. We have found for the first time that the heteroarylene methines approach this limit within a factor of 2 while even the best known molecule so far falls short of this limit by a factor of 30.

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Acknowledgments

The corresponding author acknowledges the financial support by the University Grants Commission (UGC), Government of India for this research work.

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Authors and Affiliations

  1. Department of Physics, Indian Institute of Technology, Bombay, Powai, Mumbai, 400076, India

    B. Bhushan, T. Kundu & B. P. Singh

  2. Department of Chemistry, Indian Institute of Technology, Bombay, Powai, Mumbai, 400076, India

    S. K. Kumar & S. S. Talwar

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  1. B. Bhushan
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  2. S. K. Kumar
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  3. S. S. Talwar
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  4. T. Kundu
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  5. B. P. Singh
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Correspondence to B. Bhushan.

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Bhushan, B., Kumar, S.K., Talwar, S.S. et al. Nonlinear optical properties of novel tunable, one dimensional molecular superlattice polymers (heteroarylene methines) containing alternating aromatic and quinoid segments. Appl. Phys. B 109, 201–209 (2012). https://doi.org/10.1007/s00340-012-5199-y

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