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Spectra-Orthogonal Optical Anisotropy in Wafer-Scale Molecular Crystal Monolayers

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    Spectra-Orthogonal Optical Anisotropy in Wafer-Scale Molecular Crystal Monolayers
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    • Tomojit Chowdhury
      Tomojit Chowdhury
      Department of Chemistry, University of Chicago, Chicago, Illinois 60637, United States
      The James Frank Institute, University of Chicago, Chicago, Illinois 60637, United States
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      Orcidhttps://orcid.org/0000-0002-6841-0642
    • Fauzia Mujid
      Fauzia Mujid
      Department of Chemistry, University of Chicago, Chicago, Illinois 60637, United States
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    • Zehra Naqvi
      Zehra Naqvi
      Pritzker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60637, United States
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    • Ariana Ray
      Ariana Ray
      Department of Physics, School of Applied and Engineering Physics, Cornell University, Ithaca, New York 14853, United States
      More by Ariana Ray
    • Ce Liang
      Ce Liang
      Pritzker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60637, United States
      More by Ce Liang
      Orcidhttps://orcid.org/0000-0001-8085-1558
    • David A. Muller
      David A. Muller
      Department of Physics, School of Applied and Engineering Physics, Cornell University, Ithaca, New York 14853, United States
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    • Nathan P. Guisinger
      Nathan P. Guisinger
      Center for Nanoscale Materials, Argonne National Laboratory, Argonne, Illinois 60439, United States
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      Orcidhttps://orcid.org/0000-0001-7437-2331
    • Jiwoong Park*
      Jiwoong Park
      Department of Chemistry, University of Chicago, Chicago, Illinois 60637, United States
      The James Frank Institute, University of Chicago, Chicago, Illinois 60637, United States
      Pritzker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60637, United States
      *Email: [email protected]
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    Nano Letters

    Cite this: Nano Lett. 2025, 25, 14, 5852–5859
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    https://doi.org/10.1021/acs.nanolett.5c00731
    Published March 25, 2025
    Copyright © 2025 American Chemical Society
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    Abstract

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    Controlling the spectral and polarization response of two-dimensional (2D) crystals is vital for developing ultrathin platforms for compact optoelectronic devices. However, independently tuning optical anisotropy and spectral response remains challenging in conventional semiconductors due to the intertwined nature of their lattice and electronic structures. Here, we report spectra-orthogonal optical anisotropy─where polarization anisotropy is tuned independently of spectral response─in wafer-scale, one-atom-thick 2D molecular crystal (2DMC) monolayers synthesized on monolayer transition-metal dichalcogenide (TMD) crystals. Utilizing the concomitant spectral consistency and structural tunability of perylene derivatives, we demonstrate tunable optical polarization anisotropy in 2DMCs with similar spectral profiles, as confirmed by room-temperature scanning tunneling microscopy and cross-polarized reflectance microscopy. Additional angle-dependent analysis of the single-crystal and polycrystalline molecular domains reveals an epitaxial relationship between the 2DMC and TMD. Our results establish a scalable, molecule-based 2D crystalline platform for unique and tunable functionalities unattainable in covalent 2D solids.

    Copyright © 2025 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.nanolett.5c00731.

    • Video of an θ-dependent ΔR/R map at the molecular absorption energy (MP4)

    • Video of an θ-dependent ΔR/R map at the WS2 excitation energy (MP4)

    • Description of the vector model and anisotropy (Discussion section), additional experimental data to support generality of synthesis, optical measurement methods, and domain structure analysis (Figures section), and tables (Tables section). (PDF)

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    Nano Letters

    Cite this: Nano Lett. 2025, 25, 14, 5852–5859
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.nanolett.5c00731
    Published March 25, 2025
    Copyright © 2025 American Chemical Society
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