School of Chemistry - Research Publications

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    A General Method for Direct Assembly of Single Nanocrystals
    Zhang, H ; Liu, Y ; Ashokan, A ; Gao, C ; Dong, Y ; Kinnear, C ; Kirkwood, N ; Zaman, S ; Maasoumi, F ; James, TD ; Widmer-Cooper, A ; Roberts, A ; Mulvaney, P (WILEY-V C H VERLAG GMBH, 2022-07)
    Abstract Controlled nanocrystal assembly is a pre‐requisite for incorporation of these materials into solid state devices. Many assembly methods have been investigated which target precise nanocrystal positioning, high process controllability, scalability, and universality. However, most methods are unable to achieve all of these goals. Here, surface templated electrophoretic deposition (STED) is presented as a potential assembly method for a wide variety of nanocrystals. Controlled positioning and deposition of a wide range of nanocrystals into arbitrary spatial arrangements − including gold nanocrystals of different shapes and sizes, magnetic nanocrystals, fluorescent organic nanoparticles, and semiconductor quantum dots − is demonstrated. Nanoparticles with diameters <10 nm are unable to be deposited due to their low surface charge and strong Brownian motion (low Péclet number). It is shown that this limit can be circumvented by forming clusters of nanocrystals or by silica coating nanocrystals to increase their effective size.
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    Direct Assembly of Large Area Nanoparticle Arrays
    Zhang, H ; Cadusch, J ; Kinnear, C ; James, T ; Roberts, A ; Mulvaney, P (AMER CHEMICAL SOC, 2018-08)
    A major goal of nanotechnology is the assembly of nanoscale building blocks into functional optical, electrical, or chemical devices. Many of these applications depend on an ability to optically or electrically address single nanoparticles. However, positioning large numbers of single nanocrystals with nanometer precision on a substrate for integration into solid-state devices remains a fundamental roadblock. Here, we report fast, scalable assembly of thousands of single nanoparticles using electrophoretic deposition. We demonstrate that gold nanospheres down to 30 nm in size and gold nanorods <100 nm in length can be assembled into predefined patterns on transparent conductive substrates within a few seconds. We find that rod orientation can be preserved during deposition. As proof of high fidelity scale-up, we have created centimeter scale patterns comprising more than 1 million gold nanorods.
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    Directed Chemical Assembly of Single and Clustered Nanoparticles with Silanized Templates
    Kinnear, C ; Cadusch, J ; Zhang, H ; Lu, J ; James, TD ; Roberts, A ; Mulvaney, P (AMER CHEMICAL SOC, 2018-06-26)
    The assembly of nanoscale materials into arbitrary, organized structures remains a major challenge in nanotechnology. Herein, we report a general method for creating 2D structures by combining top-down lithography with bottom-up chemical assembly. Under optimal conditions, the assembly of gold nanoparticles was achieved in less than 30 min. Single gold nanoparticles, from 10 to 100 nm, can be placed in predetermined patterns with high fidelity, and higher-order structures can be generated consisting of dimers or trimers. It is shown that the nanoparticle arrays can be transferred to, and embedded within, polymer films. This provides a new method for the large-scale fabrication of nanoparticle arrays onto diverse substrates using wet chemistry.
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    Concealed Structural Colors Uncovered by Light Scattering
    Akinoglu, EM ; Song, J ; Kinnear, C ; Xue, Y ; Zhang, H ; Roberts, A ; Koehler, J ; Mulvaney, P (WILEY-V C H VERLAG GMBH, 2020-11)
    Abstract Unusual structural colors are demonstrated in thin‐film coatings due to a combination of optical interference and light scattering effects. These vivid colors are concealed under ambient illumination but can be observed when light is reflected from the film surface. The origin of the effect is explored computationally and it is shown that, in thin‐films of lossless dielectrics coated on near‐perfect conductors, incident electromagnetic waves form standing waves. Electric field intensities at the thin film interfaces are maximized for wavelengths that fulfil destructive interference conditions, while nanoscale roughness can enhance scattering at these boundaries. The interplay of these two factors yields vivid, thickness‐dependent colors. This approach increases the repertoire of optical effects and perceived colors in thin coatings. When combined with traditional thin‐film interference colours, dichromatic images with distinctly changing colors can be generated, which can function as a covert, optical security feature.
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    Ultrathin Ceramic Membranes as Scaffolds for Functional Cell Coculture Models on a Biomimetic Scale
    Jud, C ; Ahmed, S ; Mueller, L ; Kinnear, C ; Vanhecke, D ; Umehara, Y ; Frey, S ; Liley, M ; Angeloni, S ; Petri-Fink, A ; Rothen-Rutishauser, B (MARY ANN LIEBERT, INC, 2015-12-01)
    Epithelial tissue serves as an interface between biological compartments. Many in vitro epithelial cell models have been developed as an alternative to animal experiments to answer a range of research questions. These in vitro models are grown on permeable two-chamber systems; however, commercially available, polymer-based cell culture inserts are around 10 μm thick. Since the basement membrane found in biological systems is usually less than 1 μm thick, the 10-fold thickness of cell culture inserts is a major limitation in the establishment of realistic models. In this work, an alternative insert, accommodating an ultrathin ceramic membrane with a thickness of only 500 nm (i.e., the Silicon nitride Microporous Permeable Insert [SIMPLI]-well), was produced and used to refine an established human alveolar barrier coculture model by both replacing the conventional inserts with the SIMPLI-well and completing it with endothelial cells. The structural-functional relationship of the model was evaluated, including the translocation of gold nanoparticles across the barrier, revealing a higher translocation if compared to corresponding polyethylene terephthalate (PET) membranes. This study demonstrates the power of the SIMPLI-well system as a scaffold for epithelial tissue cell models on a truly biomimetic scale, allowing construction of more functionally accurate models of human biological barriers.
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    An in vitro testing strategy towards mimicking the inhalation of high aspect ratio nanoparticles
    Endes, C ; Schmid, O ; Kinnear, C ; Mueller, S ; Camarero-Espinosa, S ; Vanhecke, D ; Foster, EJ ; Petri-Fink, A ; Rothen-Rutishauser, B ; Weder, C ; Clift, MJD (BMC, 2014-09-23)
    BACKGROUND: The challenge remains to reliably mimic human exposure to high aspect ratio nanoparticles (HARN) via inhalation. Sophisticated, multi-cellular in vitro models are a particular advantageous solution to this issue, especially when considering the need to provide realistic and efficient alternatives to invasive animal experimentation for HARN hazard assessment. By incorporating a systematic test-bed of material characterisation techniques, a specific air-liquid cell exposure system with real-time monitoring of the cell-delivered HARN dose in addition to key biochemical endpoints, here we demonstrate a successful approach towards investigation of the hazard of HARN aerosols in vitro. METHODS: Cellulose nanocrystals (CNCs) derived from cotton and tunicates, with differing aspect ratios (~9 and ~80), were employed as model HARN samples. Specifically, well-dispersed and characterised CNC suspensions were aerosolised using an "Air Liquid Interface Cell Exposure System" (ALICE) at realistic, cell-delivered concentrations ranging from 0.14 to 1.57 μg/cm2. The biological impact (cytotoxicity, oxidative stress levels and pro-inflammatory effects) of each HARN sample was then assessed using a 3D multi-cellular in vitro model of the human epithelial airway barrier at the air liquid interface (ALI) 24 hours post-exposure. Additionally, the testing strategy was validated using both crystalline quartz (DQ12) as a positive particulate control in the ALICE system and long fibre amosite asbestos (LFA) to confirm the susceptibility of the in vitro model to a fibrous insult. RESULTS: A rapid (≤ 4 min), controlled nebulisation of CNC suspensions enabled a dose-controlled and spatially homogeneous CNC deposition onto cells cultured under ALI conditions. Real-time monitoring of the cell-delivered CNC dose with a quartz crystal microbalance was accomplished. Independent of CNC aspect ratio, no significant cytotoxicity (p>0.05), induction of oxidative stress, or (pro)-inflammatory responses were observed up to the highest concentration of 1.57 μg/cm2. Both DQ12 and LFA elicited a significant (p<0.05) pro-inflammatory response at sub-lethal concentrations in vitro. CONCLUSION: In summary, whilst the present study highlights the benign nature of CNCs, it is the advanced technological and mechanistic approach presented that allows for a state of the art testing strategy to realistically and efficiently determine the in vitro hazard concerning inhalation exposure of HARN.
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    Direct Assembly of Vertically Oriented, Gold Nanorod Arrays
    Zhang, H ; Liu, Y ; Shahidan, MFS ; Kinnear, C ; Maasoumi, F ; Cadusch, J ; Akinoglu, EM ; James, TD ; Widmer-Cooper, A ; Roberts, A ; Mulvaney, P (WILEY-V C H VERLAG GMBH, 2021-02-03)
    Although many nanoscale materials such as quantum dots and metallic nanocrystals exhibit size dependent optical properties, it has been difficult to incorporate them into optical or electronic devices because there are currently no methods for precise, large‐scale deposition of single nanocrystals. Of particular interest is the need to control the orientation of single nanocrystals since the optical properties are usually strongly anisotropic. Here a method based on electrophoretic deposition (EPD) is reported to precisely assemble vertically oriented, single gold nanorods. It is demonstrated that the orientation of gold nanorods during deposition is controlled by the electric dipole moment induced along the rod by the electric field. Dissipative particle dynamics simulations indicate that the magnitude of this dipole moment is dominated by the polarizability of the solution phase electric double layer around the nanorod. The resulting vertical gold nanorod arrays exhibit reflected colors due to selective excitation of the transverse surface plasmon mode. The EPD method allows assembly of arrays with a density of over one million, visually resolvable, vertical nanorods per square millimeter.