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Generation of Hot Electrons with Chiral Metamaterial Perfect Absorbers: Giant Optical Chirality for Polarization-Sensitive Photochemistry

  • Wenhao Wang
    Wenhao Wang
    Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
    More by Wenhao Wang
  • Lucas V. Besteiro
    Lucas V. Besteiro
    Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
    Centre Énergie Matériaux et Télécommunications, Institut National de la Recherche Scientifique, Varennes, Quebec J3X 1S2, Canada
  • Tianji Liu
    Tianji Liu
    Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
    Graduate School of Engineering, Osaka University, 2-1 Yamadaoka, Suita, Osaka 565-0871, Japan
    More by Tianji Liu
  • Cuo Wu
    Cuo Wu
    Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
    More by Cuo Wu
  • Jiachen Sun
    Jiachen Sun
    Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
    More by Jiachen Sun
  • Peng Yu
    Peng Yu
    Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
    More by Peng Yu
  • Le Chang
    Le Chang
    Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
    More by Le Chang
  • Zhiming Wang*
    Zhiming Wang
    Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
    *E-mail: [email protected]
    More by Zhiming Wang
  • , and 
  • Alexander O. Govorov*
    Alexander O. Govorov
    Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
    Department of Physics and Astronomy, Ohio University, Athens, Ohio 45701, United States
    *E-mail: [email protected]
Cite this: ACS Photonics 2019, 6, 12, 3241–3252
Publication Date (Web):October 31, 2019
Copyright © 2019 American Chemical Society

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    Abstract Image

    Chiral plasmonic metamaterials have shown very interesting possibilities as chiral optical absorbers for circularly polarized light detection, as their optical response can be manipulated through the careful design of their geometry. Exhibiting the generation of hot electrons, chiral plasmonic nanostructures can be potentially used for polarization-sensitive photochemistry and chiral photocatalysis, in which the excited hot electrons induce surface reactions. In this study, we show that chiral metamaterial perfect absorbers (MMPAs) can be utilized for plasmon-induced polarization-sensitive photochemistry involving hot electrons, with extremely strong differential chiral responses. The calculated nearly perfect optical absorption (∼98%) of metamaterials demonstrate that the MMPAs can strongly absorb the photons and direct a significant part of the radiant energy to the generation of energetic (hot) carriers. Through the elaborate design of the plasmonic antenna geometry, we theoretically present a MMPA exhibiting a very large circular dichroism in its optical response. In addition, the greatly asymmetric electromagnetic field enhancement response of the MMPA to left and right circularly polarized light leads to a large chiral effect in the hot electron generation. In our calculations with the optimized designs, the g-factor reaches a value of 1.52, close to the theoretical upper limit of 2, higher than that of chiral colloidal nanocrystals with plasmonic resonances and much higher than for any chiral molecules. The remarkably strong chiral effect in hot electron generation, predicted in our study, suggests that plasmonic MMPAs can be used in polarization-sensitive photochemical applications and for photodetection.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsphotonics.9b01180.

    • Additional details about the effect of the edges of the nanoantennas on the optical response of the metamaterials; detailed description of the proposed metamaterials; magnetic fields; Ratehigh-energy for different surface areas of RH metamaterials; discussion on the effect of different heights for the potential barrier formed between Au–TiO2 and Au–water interfaces on the Ratehigh-energy; Ratehigh-energy,wall spectra of the LH metamaterial for different periodicities (PDF)

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