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Synthesis of Gold NPs-Containing Thin Films from Metal Salt Injection in Ar or Ar–NH3 DBDs

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Abstract

This study focuses on metal/polymer nanocomposite thin films made by atmospheric pressure Plasma-Enhanced Chemical Vapor Deposition. The aerosol of isopropanol-dissolved tetrachloroauric acid (HAuCl4:3H2O gold salt) is injected in a dielectric barrier discharge to synthesize plasmonic nanocomposite thin films. Argon is used as carrier gas with or without 133 ppm addition of ammonia (NH3) to respectively get or not a Penning mixture. Results show that NH3 largely influences the salt reduction and thin film properties. According to the aerosol characterization, the size distribution at the plasma entrance supports that isopropanol mainly evaporates before injection in the plasma. The salt initially dissolved in each droplet precipitates during evaporation before injection as solid nanoparticles of about 30 nm diameter with eventual traces of solvent. Then, the nanocomposite thins film are studied. Optical properties, as plasmonic resonance, are characterized by UV–visible absorption spectroscopy. The chemical composition is analyzed using X-ray photoelectron spectroscopy and Raman spectroscopy, complemented by X-ray diffraction analysis as well as chemical mapping obtained by Energy dispersive spectroscopy coupled to scanning electron microscopy (SEM) operating in Scanning Transmission Electron Microscopy mode. Additionally, the morphology of the deposits is investigated by atomic force microscopy and SEM, highlighting the influence of NH3 gas on the film nature and therefore its role in the overall deposition process. Finally, optical emission spectroscopy of the plasma gives clue to better understand the effect of NH3. The overall results show that the salt nanoparticles are reduced in the plasma phase leading to non-aggregated metal Au NPs embedded in a carbon-based matrix formed by isopropanol polymerization. The presence of NH3 in the plasma unambiguously decreases the salt reduction and affects the thin film properties, consequently changing their plasmonic response related to the size, concentration, and composition of the embedded NPs.

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Acknowledgements

The authors thank the Agence Nationale de la Recherche (ANR) for the financial support of the PLASSEL project (ANR-21-CE08-0038) and the SEAM Labex (ANR-11-LBX-086, ANR-11-IDEX-0502). R. Rincón was supported by the European Union-NextGenerationEU and the Spanish Ministerio de Universidades (Plan de Recuperacion, Transformación y Resiliencia).

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Authors and Affiliations

  1. Laboratoire Procédés Matériaux et Énergie Solaire (PROMES, CNRS), UPR-8521, Rambla de la thermodynamique, 66100, Perpignan, France

    Alexandre Perdrau, Noémi Barros, Rocío Rincón, Hervé Glénat, Béatrice Plujat & Françoise Massines

  2. Université Perpignan Via Domitia (UPVD), 52 Av Paul Alduy, 66100, Perpignan, France

    Alexandre Perdrau, Noémi Barros & Béatrice Plujat

  3. Laboratory of Innovation in Plasmas (LIPs), Universidad de Córdoba, 14071, Córdoba, Spain

    Rocío Rincón

  4. Laboratoire Interface Traitement Organisation et Dynamique des Systèmes (ITODYS), CNRS, UMR-7086, Université Paris Cité, 15 Rue Jean-Antoine de Baïf, 75205, Paris, France

    Stéphanie Truong, Sarra Gam Derouich, Xiaonan Sun, Philippe Decorse, Sophie Nowak & Souad Ammar

  5. Laboratoire de Physique des Gaz et des Plasmas, (LPGP CNRS-Université Paris-Saclay), UMR-8578, Université Paris-Saclay, Bat 210, Rue Becquerel, 91405, Orsay Cedex, France

    Jean-Pascal Borra

  6. Institute of Nanotechnology (NANOTEC), National Research Council (CNR), Bari, Italy

    Fiorenza Fanelli

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  1. Alexandre Perdrau
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Contributions

This work was carried out as part of a collaborative project involving AP, NB, RR, HG, ST, SGD, XS, PD, SN, BP, SA, JPB, FF, FM. AP, NB, RR, HG, ST, SGD, XS, PD, SN, BP, SA, JPB, FF, FM actively contributed to the writing of the paper. FM, NB, RR, FF, BP supervised the whole work and participated in the whole results analysis and paper writing. FF, BP and AP find the proper parameter of use of the AP-PECVD set-up. AP contributed to the whole experimental work. He specifically took in charge all the samples deposit by AP-PECVD, and thin film UV-vis and plasma emission spectroscopy measurements made in PROMES. He also participated in aerosols and samples characterization. JPB brought his expertise on aerosols and all aerosol characterization were done in his lab. NB specifically made all the calculations relative to the NPs and UV-Vis spectra analysis. RR specifically made emission spectroscopy spectra analysis as well as XPS results analysis. PD, SGD, HG, SN, ST made XPS, SEM-EDS, AFM (made in PROMES), XRD, Raman measurements and results analysis respectively. SA supervised XPS, SEM, EDS, XRD, AFM and Raman characterization and results analysis made in ITODYS correlating the obtained results to each other.

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Correspondence to Françoise Massines.

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Perdrau, A., Barros, N., Rincón, R. et al. Synthesis of Gold NPs-Containing Thin Films from Metal Salt Injection in Ar or Ar–NH3 DBDs. Plasma Chem Plasma Process 43, 1749–1772 (2023). https://doi.org/10.1007/s11090-023-10400-4

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