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Mechanistic Insight into Solution-Based Atomic Layer Deposition of CuSCN Provided by In Situ and Ex Situ Methods

Hilpert, Felix; Liao, Pei-Chun; Franz, Evanie; Koch, Vanessa M.; Fromm, Lukas; Topraksal, Ece; Görling, Andreas; Smith, Ana-Sunc̆ana; Barr, Maïssa K. S.; Bachmann, Julien; Brummel, Olaf; Libuda, Jörg (2023) Mechanistic Insight into Solution-Based Atomic Layer Deposition of CuSCN Provided by In Situ and Ex Situ Methods. ACS Applied Materials & Interfaces, 15 (15). pp. 19536-19544. ISSN 1944-8244

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Solution-based atomic layer deposition (sALD) processes enable the preparation of thin films on nanostructured surfaces while controlling the film thickness down to a monolayer and preserving the homogeneity of the film. In sALD, a similar operation principle as in gas-phase ALD is used, however, with a broader range of accessible materials and without requiring expensive vacuum equipment. In this work, a sALD process was developed to prepare CuSCN on a Si substrate using the precursors CuOAc and LiSCN. The film growth was studied by ex situ atomic force microscopy (AFM), analyzed by a neural network (NN) approach, ellipsometry, and a newly developed in situ infrared (IR) spectroscopy experiment in combination with density functional theory (DFT). In the self-limiting sALD process, CuSCN grows on top of an initially formed two-dimensional (2D) layer as three-dimensional spherical nanoparticles with an average size of ∼25 nm and a narrow particle size distribution. With increasing cycle number, the particle density increases and larger particles form via Ostwald ripening and coalescence. The film grows preferentially in the β-CuSCN phase. Additionally, a small fraction of the α-CuSCN phase and defect sites form.

Item Type: Article
Uncontrolled Keywords: solution atomic layer ; deposition liquid phase ;in situ IR spectroscopy ; atomic force microscopy ; copper thiocyanate ; neural network density ; functional theory ; liquid atomic layer deposition
Divisions: Division of Physical Chemistry
Depositing User: Ana Sunčana Smith
Date Deposited: 27 Jun 2023 13:37
DOI: 10.1021/acsami.2c16943

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