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1. Chelating Agent Functionalized Substrates for the Formation of Thick Films via Electrophoretic Deposition

   https://doi.org/10.3389/fchem.2021.703528  

   Mills, Sara C.; Starr, Natalie E.; Bohannon, Nicholas J.; Andrew, Jennifer S. (June 2021, Frontiers in Chemistry)

   null (Ed.)

   Incorporating nanoparticles into devices for a wide range of applications often requires the formation of thick films, which is particularly necessary for improving magnetic power storage, microwave properties, and sensor performance. One approach to assembling nanoparticles into films is the use of electrophoretic deposition (EPD). This work seeks to develop methods to increase film thickness and stability in EPD by increasing film-substrate interactions via functionalizing conductive substrates with various chelating agents. Here, we deposited iron oxide nanoparticles onto conductive substrates functionalized with three chelating agents with different functional moieties and differing chelating strengths. We show that increasing chelating strength can increase film-substrate interactions, resulting in thicker films when compared to traditional EPD. Results will also be presented on how the chelating strength relates to film formation as a function of deposition conditions. Yield for EPD is influenced by deposition conditions including applied electric field, particle concentration, and deposition time. This work shows that the functionalization of substrates with chelating agents that coordinate strongly with nanoparticles (phosphonic acid and dopamine) overcome parameters that traditionally hinder the deposition of thicker and more stable films, such as applied electric field and high particle concentration. We show that functionalizing substrates with chelating agents is a promising method to fabricate thick, stable films of nanoparticles deposited via EPD over a larger processing space by increasing film-substrate interactions. 

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2. Film Thickness Dependence of Surface and Internal Morphology Evolution in Polymer-Grafted Nanocomposites

   https://doi.org/10.1021/acs.macromol.4c00854  

   Zhang, Aria C; Ohno, Kohji; Composto, Russell J (July 2024, Macromolecules)

   This study investigates the interplay between film thickness and the surface and internal morphologies in polymer nanocomposite (PNC) films. The PNC is 25 wt.% poly(methyl methacrylate)-grafted silica nanoparticles (NPs) in poly(styrene-ran-acrylonitrile) annealed in the two-phase region. At greatest confinement (120 nm), NP surface density remains constant and lateral phase separation is inhibited upon annealing. For thicker films (240 nm to 1400 nm), surface density increases with time before approaching ca. 740 NP/μm2, consistent with 2D random close packing. Moreover, lateral domain growth exhibits a dimensional crossover as thickness increases from 𝑡 to , consistent with domain coalescence. Water contact angles 1/2 𝑡1/3 decrease upon annealing in agreement with the lateral domain composition. For thickest films (1400 nm to 4000 nm), a morphology map summarizes the distinct internal arrangements of NPs: disordered aggregates, continuous vertical pillars, discrete vertical pillars, isolated domains, and random networks. This study of PNC films provides guidance for controlling surface and bulk structure which can lead to improved barrier, mechanical and transport properties. 

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3. A Hybrid Pulsed Laser Deposition Approach to Grow Thin Films of Chalcogenides

   https://doi.org/10.1002/adma.202312620  

   Surendran, Mythili; Singh, Shantanu; Chen, Huandong; Wu, Claire; Avishai, Amir; Shao, Yu‐Tsun; Ravichandran, Jayakanth (February 2024, Advanced Materials)

   Abstract Vapor‐pressure mismatched materials such as transition metal chalcogenides have emerged as electronic, photonic, and quantum materials with scientific and technological importance. However, epitaxial growth of vapor‐pressure mismatched materials are challenging due to differences in the reactivity, sticking coefficient, and surface adatom mobility of the mismatched species constituting the material, especially sulfur containing compounds. Here, a novel approach is reported to grow chalcogenides—hybrid pulsed laser deposition—wherein an organosulfur precursor is used as a sulfur source in conjunction with pulsed laser deposition to regulate the stoichiometry of the deposited films. Epitaxial or textured thin films of sulfides with variety of structure and chemistry such as alkaline metal chalcogenides, main group chalcogenides, transition metal chalcogenides, and chalcogenide perovskites are demonstrated, and structural characterization reveal improvement in thin film crystallinity, and surface and interface roughness compared to the state‐of‐the‐art. The growth method can be broadened to other vapor‐pressure mismatched chalcogenides such as selenides and tellurides. This work opens up opportunities for broader epitaxial growth of chalcogenides, especially sulfide‐based thin film technological applications. 

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4. Rapid Color‐Switching of MnO ₂ Hollow‐Nanosphere Films in Dynamic Water Vapor for Reversible Optical Encryption

   https://doi.org/10.1002/smll.202204484  

   Chen, Yibo; Zuo, Zhi‐Han; Liu, Zhao‐Qing; Yin, Yadong (October 2022, Small)

   Abstract Drop‐casting manganese oxide (MnO₂) hollow nanospheres synthesized via a simple surface‐initiated redox route produces thin films exhibiting angle‐independent structural colors. The colors can rapidly change in response to high‐humidity dynamic water vapor (relative humidity > 90%) with excellent reversibility. When the film is triggered by dynamic water vapor with a relative humidity of ≈100%, the color changes with an optimal wavelength redshift of ≈60 nm at ≈600 ms while there is no shift under static water vapor. The unique selective response originates from the nanoscale porosity formed in the shells by randomly stacked MnO₂nanosheets, which enhances the capillary condensation of dynamic water vapor and promotes the change of their effective refractive index for rapid color switching. The repeated color‐switching tests over 100 times confirm the durability and reversibility of the MnO₂film. The potential of these films for applications in anti‐counterfeiting and information encryption is further demonstrated by reversible encoding and decoding initiated exclusively by exposure to human breath. 

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5. Temperature-dependent morphology and composition of ultra-thin GeSn epilayers prepared by remote plasma enhanced chemical vapor deposition

   https://doi.org/10.1116/6.0003445  

   Jiang, Jiechao; Chetuya, Nonso Martin; Meletis, Efstathios I; Ngai, Joseph H; Grzybowski, Gordon J; Claflin, Bruce (May 2024, Journal of Vacuum Science & Technology B)

   Two distinct ultra-thin Ge1−xSnx (x ≤ 0.1) epilayers were deposited on (001) Si substrates at 457 and 313 °C through remote plasma-enhanced chemical vapor deposition. These films are considered potential initiation layers for synthesizing thick epitaxial GeSn films. The GeSn film deposited at 313 °C has a thickness of 10 nm and exhibits a highly epitaxial continuous structure with its lattice being compressed along the interface plane to coherently match Si without mismatch dislocations. The GeSn film deposited at 457 °C exhibits a discrete epitaxial island-like morphology with a peak height of ∼30 nm and full-width half maximum (FWHM) varying from 20 to 100 nm. GeSn islands with an FWHM smaller than 20 nm are defect free, whereas those exceeding 25 nm encompass nanotwins and/or stacking faults. The GeSn islands form two-dimensional modulated superlattice structures at the interface with Si. The GeSn film deposited at 457 °C possesses a lower Sn content compared to the one deposited at lower temperature. The potential impact of using these two distinct ultra-thin layers as initiation layers for the direct growth of thicker GeSn epitaxial films on (001) Si substrates is discussed. 

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