Extreme Polarization Anisotropy in Resonant Third‐Harmonic Generation from Aligned Carbon Nanotube Films

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  • Song Zhu
    School of Electrical and Electronic Engineering Nanyang Technological University Singapore 639798 Singapore
  • Wenkai Li
    State Key Laboratory of High Field Laser Physics Shanghai Institute of Optics and Fine Mechanics Chinese Academy of Sciences Shanghai 201800 China
  • Shengjie Yu
    Department of Electrical and Computer Engineering Rice University Houston TX 77005 USA
  • Natsumi Komatsu
    Department of Electrical and Computer Engineering Rice University Houston TX 77005 USA
  • Andrey Baydin
    Department of Electrical and Computer Engineering Rice University Houston TX 77005 USA
  • Fakun Wang
    School of Electrical and Electronic Engineering Nanyang Technological University Singapore 639798 Singapore
  • Fangyuan Sun
    School of Electrical and Electronic Engineering Nanyang Technological University Singapore 639798 Singapore
  • Chongwu Wang
    School of Electrical and Electronic Engineering Nanyang Technological University Singapore 639798 Singapore
  • Wenduo Chen
    School of Electrical and Electronic Engineering Nanyang Technological University Singapore 639798 Singapore
  • Chuan Seng Tan
    School of Electrical and Electronic Engineering Nanyang Technological University Singapore 639798 Singapore
  • Houkun Liang
    School of Electronics and Information Engineering Sichuan University Chengdu Sichuan 610064 China
  • Yohei Yomogida
    Department of Physics Tokyo Metropolitan University Hachioji Tokyo 192‑0397 Japan
  • Kazuhiro Yanagi
    Department of Physics Tokyo Metropolitan University Hachioji Tokyo 192‑0397 Japan
  • Junichiro Kono
    Department of Electrical and Computer Engineering Rice University Houston TX 77005 USA
  • Qi Jie Wang
    School of Electrical and Electronic Engineering Nanyang Technological University Singapore 639798 Singapore
  • School of Electrical and Electronic Engineering
  • School of Physical and Mathematical Sciences

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<jats:title>Abstract</jats:title><jats:p>Carbon nanotubes (CNTs) possess extremely anisotropic electronic, thermal, and optical properties owing to their 1D character. While their linear optical properties have been extensively studied, nonlinear optical processes, such as harmonic generation for frequency conversion, remain largely unexplored in CNTs, particularly in macroscopic CNT assemblies. In this work, macroscopic films of aligned and type‐separated (semiconducting and metallic) CNTs are synthesized and polarization‐dependent third‐harmonic generation (THG) from the films with fundamental wavelengths ranging from 1.5 to 2.5 µm is studied. Both films exhibited strongly wavelength‐dependent, intense THG signals, enhanced through exciton resonances, and third‐order nonlinear optical susceptibilities of 2.50 × 10<jats:sup>−19</jats:sup> m<jats:sup>2</jats:sup> V<jats:sup>−2</jats:sup> (semiconducting CNTs) and 1.23 × 10<jats:sup>−19</jats:sup> m<jats:sup>2</jats:sup> V<jats:sup>−2</jats:sup> (metallic CNTs), respectively are found, for 1.8 µm excitation. Further, through systematic polarization‐dependent THG measurements, the values of all elements of the susceptibility tensor are determined, verifying the macroscopically 1D nature of the films. Finally, polarized THG imaging is performed to demonstrate the nonlinear anisotropy in the large‐size CNT film with good alignment. These findings promise applications of aligned CNT films in mid‐infrared frequency conversion, nonlinear optical switching, polarized pulsed lasers, polarized long‐wave detection, and high‐performance anisotropic nonlinear photonic devices.</jats:p>

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