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Mechanisms of the anomalous Pockels effect in bulk water

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Abstract

The “anomalous” Pockels effect is a phenomenon that a light beam passing between two electrodes in an aqueous electrolyte solution is deflected by an AC voltage applied between the electrodes: the deflection angle is proportional to the voltage such that the incident beam alternately changes its direction. This phenomenon, the Pockels effect in bulk water, apparently contradicts what is believed in nonlinear optics, i.e., macroscopic inversion symmetry should be broken for the second-order nonlinear optical effect to occur such as the first-order electro-optic effect, i.e., the Pockels effect. To clarify the underlying mechanism, the dependence of the effect on the electrode material is investigated to find that the Pockels coefficient with Pt electrodes is two orders of magnitude smaller than with indium tin oxide (ITO) electrodes. It is experimentally confirmed that the Pockels effect of interfacial water in the electric double layer (EDL) on these electrodes shows an electrode dependence similar to the effect in bulk water while the effects depend on the frequency of the AC voltage such that the interfacial signal decreases with frequency but the bulk signal increases with frequency up to 221 Hz. These experimental results lead to a conclusion that the beam deflection is caused by the refractive index gradient in the bulk water region, which is formed transiently by the Pockels effect of interfacial water in the EDL when an AC electric field is applied. The refractive index gradient is caused by the diffuse layer spreading into the bulk region to work as a breaking factor of inversion symmetry of bulk water due to its charge-biased ionic distribution. This mechanism does not contradict the principle of nonlinear optics.

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Acknowledgements

The authors would like to thank Prof. Kiyoshi Asakawa and Prof. Yasuhiro Horiike from University of Tsukuba for their valuable comments. This work was supported by a Grant-in-Aid for Scientific Research(C) (Grant Number JP15K05134), Japan Society for the Promotion of Science (JSPS).

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Authors and Affiliations

  1. Department of Physics, Faculty of Science, Tokyo University of Science, 1-3 Kagurazaka, Shinjuku-ku, Tokyo, 162-8601, Japan

    Shunpei Yukita, Yuto Suzuki, Naoyuki Shiokawa & Eiji Tokunaga

  2. Research Center for Water Frontier Science and Technology, Tokyo University of Science, 1-3 Kagurazaka, Shinjuku-ku, Tokyo, 162-8601, Japan

    Eiji Tokunaga

  3. Advanced Ultrafast Laser Research Center and Brain Science Inspired Life Support Research Center, The University of Electro-Communications, 1-5-1 Chofugaoka, Chofu, Tokyo, 182-8585, Japan

    Takayoshi Kobayashi

  4. Advanced Ultrafast Laser Research Center, Department of Electrophysics, National Chiao-Tung University, 1001 Ta Hsinchu Rd., Hsinchu, 300, Taiwan

    Takayoshi Kobayashi

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  1. Shunpei Yukita
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  2. Yuto Suzuki
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  3. Naoyuki Shiokawa
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  4. Takayoshi Kobayashi
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  5. Eiji Tokunaga
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Correspondence to Eiji Tokunaga.

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Yukita, S., Suzuki, Y., Shiokawa, N. et al. Mechanisms of the anomalous Pockels effect in bulk water. Opt Rev 25, 205–214 (2018). https://doi.org/10.1007/s10043-018-0407-6

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  • DOI: https://doi.org/10.1007/s10043-018-0407-6

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