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90-degree optical switching of output second-harmonic light in chiral photomagnet

Nature Photonics volume 8, pages 65–71 (2014)Cite this article

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Abstract

Optical control of physical properties and functionalities is an attractive area of research in the development of advanced optical materials. Here, we report a magnet that can switch the polarization plane of light by 90° under optical stimulation. The magnet is a chiral structured iron-octacyanoniobate, and its magnetic properties can be reversibly switched by irradiating with blue and red light, which causes light-reversible spin-crossover on the iron(II) ion. Using this material, second-harmonic generation, a nonlinear optical effect, was investigated. The vertical polarization plane was switched to horizontal polarization by irradiating with blue light, and was then returned to the original vertical polarization by irradiating with red light. This phenomenon originates from alternate optical switching between crystallographic and magnetic contributions to second-harmonic generation within the magnet, where the chiral structure and photomagnetism are coupled. The observed perpendicular optical switching should encourage studies in the fields of magneto-optical memory and optoelectronic devices.

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Figure 1: Crystal structure of (±)-Fe2[Nb(CN)8](4-bromopyridine)8·2H2O.
Figure 2: Spin-crossover effect on magnetic susceptibility and spin-crossover induced SHG.
Figure 3: Photo-reversible magnetization due to light-reversible spin-crossover effect.
Figure 4: Optical switching of MSHG.

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Acknowledgements

The authors thank K. Nakagawa and K. Nakabayashi for helpful discussions. The authors also thank T. Uchiyama of JASCO Corporation for the NCD measurement. The present research was supported in part by the Core Research for Evolutional Science and Technology project of the Japan Science and Technology Agency, the Funding Program for Next Generation World-Leading Researchers from the Japan Society for the Promotion of Science (JSPS), a Grant for the Global COE Program ‘Chemistry Innovation through Cooperation of Science and Engineering’, the Advanced Photon Science Alliance from the Ministry of Education, Culture, Sports, Science & Technology (MEXT), and the Asahi Glass Foundation. The authors also recognize the Cryogenic Research Center, The University of Tokyo, and the Center for Nano Lithography & Analysis, The University of Tokyo, which are supported by MEXT. M.Y. is grateful to the Advanced Leading Graduate Course for Photon Science. A.N. is thankful to the Research Activity Start-up, and K.I. and M.Y. are grateful for a Research Fellowship for Young Scientists of JSPS.

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Authors and Affiliations

  1. Department of Chemistry, School of Science, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo, 113-0033, Japan

    Shin-ichi Ohkoshi, Shinjiro Takano, Kenta Imoto, Marie Yoshikiyo, Asuka Namai & Hiroko Tokoro

  2. CREST, JST, K's Gobancho, 7 Gobancho, Chiyoda-ku, Tokyo, 102-0076, Japan

    Shin-ichi Ohkoshi

  3. NEXT, JSPS, 5-3-1 Kojimachi, Chiyoda-ku, Tokyo, 102-0083, Japan

    Hiroko Tokoro

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  1. Shin-ichi Ohkoshi
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Contributions

S.O. designed and coordinated the study, contributed to all measurements and calculations, and wrote the manuscript. S.T. performed the synthesis, photoirradiation measurements, Mössbauer spectroscopy and SHG and MSHG measurements. K.I. conducted photoirradiation measurements, Mössbauer spectroscopy and XRD measurements. M.Y. analysed the optical properties. A.N. performed XRD measurements and analysed the MSHG tensors. H.T. carried out photoirradiation measurements, XRD measurements and SHG and MSHG measurements. All authors commented on the manuscript.

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Correspondence to Shin-ichi Ohkoshi.

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Ohkoshi, Si., Takano, S., Imoto, K. et al. 90-degree optical switching of output second-harmonic light in chiral photomagnet. Nature Photon 8, 65–71 (2014). https://doi.org/10.1038/nphoton.2013.310

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