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Chemically Driven Sintering of Colloidal Cu Nanocrystals for Multiscale Electronic and Optical Devices
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    Chemically Driven Sintering of Colloidal Cu Nanocrystals for Multiscale Electronic and Optical Devices
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    • Jun Xu
      Jun Xu
      Department of Electrical and Systems Engineering, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
      More by Jun Xu
    • Tianshuo Zhao*
      Tianshuo Zhao
      Department of Electrical and Systems Engineering, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
      *Email: [email protected]
    • Anne-Marie Zaccarin
      Anne-Marie Zaccarin
      Department of Electrical and Systems Engineering, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
    • Xingyu Du
      Xingyu Du
      Department of Electrical and Systems Engineering, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
      More by Xingyu Du
    • Shengsong Yang
      Shengsong Yang
      Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
    • Yifan Ning
      Yifan Ning
      Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
      More by Yifan Ning
    • Qiwen Xiao
      Qiwen Xiao
      Department of Materials Science and Engineering, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
      More by Qiwen Xiao
    • Shobhita Kramadhati
      Shobhita Kramadhati
      Department of Materials Science and Engineering, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
    • Yun Chang Choi
      Yun Chang Choi
      Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
    • Christopher B. Murray
      Christopher B. Murray
      Department of Materials Science and Engineering, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
      Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
    • Roy H. Olsson III
      Roy H. Olsson, III
      Department of Electrical and Systems Engineering, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
    • Cherie R. Kagan*
      Cherie R. Kagan
      Department of Electrical and Systems Engineering, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
      Department of Materials Science and Engineering, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
      Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
      *Email: [email protected]
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    ACS Nano

    Cite this: ACS Nano 2024, 18, 27, 17611–17621
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    https://doi.org/10.1021/acsnano.4c02007
    Published June 25, 2024
    Copyright © 2024 American Chemical Society

    Abstract

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    Emerging applications of Internet of Things (IoT) technologies in smart health, home, and city, in agriculture and environmental monitoring, and in transportation and manufacturing require materials and devices with engineered physical properties that can be manufactured by low-cost and scalable methods, support flexible forms, and are biocompatible and biodegradable. Here, we report the fabrication and device integration of low-cost and biocompatible/biodegradable colloidal Cu nanocrystal (NC) films through room temperature, solution-based deposition, and sintering, achieved via chemical exchange of NC surface ligands. Treatment of organic-ligand capped Cu NC films with solutions of shorter, environmentally benign, and noncorrosive inorganic reagents, namely, SCN and Cl, effectively removes the organic ligands, drives NC grain growth, and limits film oxidation. We investigate the mechanism of this chemically driven sintering by systemically varying the Cu NC size, ligand reagent, and ligand treatment time and follow the evolution of their structure and electrical and optical properties. Cl-treated, 4.5 nm diameter Cu NC films yield the lowest DC resistivity, only 3.2 times that of bulk Cu, and metal-like dielectric functions at optical frequencies. We exploit the high conductivity of these chemically sintered Cu NC films and, in combination with photo- and nanoimprint-lithography, pattern multiscale structures to achieve high-Q radio frequency (RF) capacitive sensors and near-infrared (NIR) resonant optical metasurfaces.

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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/acsnano.4c02007.

    • TEM images of 15.0 nm Cu NCs; UV–vis transmittance, FTIR absorbance, XRD, XPS, and diffuse reflectance measurements of 4.5 nm Cu NC films; AFM height profile data of 4.5 nm Cu NC films; DC sheet resistance of 15.0 nm Cu NC films; SEM images of 4.5 and 15.0 nm Cu NC films; DC resistivity data of 4.5 nm Cu NC films during air exposure; optical microscope images of Cu NC capacitors; RF capacitance data of Cu NC capacitors; dielectric function measurements and fitting results; and AFM images of Cu NC optical metasurface (PDF)

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    This article is cited by 2 publications.

    1. Shobhita Kramadhati, Yun Chang Choi, Cherie R. Kagan. Large-Area, Narrow-Gap Plasmonic Nanodimer Metasurfaces Exploiting Colloidal Nanocrystals: Promising Platforms for Refractive Index Sensing. ACS Applied Nano Materials 2025, 8 (9) , 4600-4607. https://doi.org/10.1021/acsanm.4c07056
    2. Huakang Yang, Zining Zhang, Yudong Guo, Shuwen Yuan, Xiao Liu, Dongxiang Luo, Siyu Ye. Concurrent Photocatalytic CO 2 Reduction and 1‐Phenylethanol Oxidation Regulated by Chloride Ion‐Capped CdS@Zn x Cd 1‐x S@ZnS QDs. Advanced Functional Materials 2025, https://doi.org/10.1002/adfm.202502562

    ACS Nano

    Cite this: ACS Nano 2024, 18, 27, 17611–17621
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsnano.4c02007
    Published June 25, 2024
    Copyright © 2024 American Chemical Society

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