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Gigantic optical nonlinearity in one-dimensional Mott–Hubbard insulators

Nature volume 405, pages 929–932 (2000)Cite this article

Abstract

The realization of all-optical switching, modulating and computing devices is an important goal in modern optical technology. Nonlinear optical materials with large third-order nonlinear susceptibilities (χ(3)) are indispensable for such devices, because the magnitude of this quantity dominates the device performance. A key strategy in the development of new materials with large nonlinear susceptibilities is the exploration of quasi-one-dimensional systems1,2, or ‘quantum wires’—the quantum confinement of electron–hole motion in one-dimensional space can enhance χ(3). Two types of chemically synthesized quantum wires have been extensively studied: the band insulators of silicon polymers, and Peierls insulators of π-conjugated polymers and platinum halides. In these systems, χ(3) values of 10-12 to 10-7 e.s.u. (electrostatic system of units) have been reported3,4,5,6,7. Here we demonstrate an anomalous enhancement of the third-order nonlinear susceptibility in a different category of quantum wires: one-dimensional Mott insulators of 3 d transition-metal oxides and halides. By analysing the electroreflectance spectra of these compounds, we measure χ(3) values in the range 10-8 to 10-5 e.s.u. The anomalous enhancement results from a large dipole moment between the lowest two excited states of these systems.

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Figure 1: Crystal and electronic structures of the 1D Mott insulators.
Figure 2: ε2 and Δε2 spectra of Sr 2CuO3, and [Ni(chxn)2Br]Br2 and isostructural Ni–Cl compounds.
Figure 3: ε2 and Imχ(3)(-ω;0,0,ω) spectra at 77 K of [Ni(chxn)2Br]Br2.
Figure 4: Comparison of the maximum values of |Imχ(3)(-ω;0,0,ω)| and transition dipole moments in various 1D materials.

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Acknowledgements

This work was supported by a grant-in-aid from the Ministry of Education, Science, Sports, and Culture of Japan.

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Authors and Affiliations

  1. Department of Advanced Materials Science, Graduate School of Frontier Sciences, University of Tokyo, Tokyo, 113-8656, Japan

    H. Kishida, H. Matsuzaki & H. Okamoto

  2. Structure and Transformation Group, PRESTO, Tokyo, 113-8656, Japan

    H. Okamoto

  3. Graduate School of Human Informatics, Nagoya University, Nagoya, 464-8601, Japan

    T. Manabe

  4. Department of Chemistry, Graduate School of Science, Tokyo Metropolitan University, Hachioji, Tokyo , 192-0397, Japan

    M. Yamashita

  5. Structure and Transformation Group, PRESTO, Hachioji, Tokyo, 192-0397, Japan

    M. Yamashita

  6. Department of Applied Physics, University of Tokyo, Tokyo, 113-8656, Japan

    Y. Taguchi & Y. Tokura

  7. Joint Research Center for Atom Technology (JRCAT), Tsukuba, Ibaraki, 305-8562, Japan

    Y. Tokura

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  1. H. Kishida
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  2. H. Matsuzaki
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  7. Y. Tokura
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Correspondence to H. Okamoto.

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Kishida, H., Matsuzaki, H., Okamoto, H. et al. Gigantic optical nonlinearity in one-dimensional Mott–Hubbard insulators . Nature 405, 929–932 (2000). https://doi.org/10.1038/35016036

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