| 1. |
- Aad, G, et al.
(author)
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- 2015
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swepub:Mat__t
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| 2. |
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| 3. |
- Brett, Calvin, et al.
(author)
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Water-Induced Structural Rearrangements on the Nanoscale in Ultrathin Nanocellulose Films
- 2019
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In: Macromolecules. - : American Chemical Society (ACS). - 0024-9297 .- 1520-5835. ; 52:12, s. 4721-4728
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Journal article (peer-reviewed)abstract
- Many nanoscale biopolymer building blocks with defect-free molecular structure and exceptional mechanical properties have the potential to surpass the performance of existing fossil-based materials with respect to barrier properties, load-bearing substrates for advanced functionalities, as well as light-weight construction. Comprehension and control of performance variations of macroscopic biopolymer materials caused by humidity-driven structural changes at the nanoscale are imperative and challenging. A long-lasting challenge is the interaction with water molecules causing reversible changes in the intrinsic molecular structures that adversely affects the macroscale performance. Using in situ advanced X-ray and neutron scattering techniques, we reveal the structural rearrangements at the nanoscale in ultrathin nanocellulose films with humidity variations. These reversible rearrangements are then correlated with wettability that can be tuned. The results and methodology have general implications not only on the performance of cellulose-based materials but also for hierarchical materials fabricated with other organic and inorganic moisture-sensitive building blocks.
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| 4. |
- Cao, Wei, et al.
(author)
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Self-Assembly of Large Magnetic Nanoparticles in Ultrahigh Molecular Weight Linear Diblock Copolymer Films
- 2020
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In: ACS Applied Materials and Interfaces. - : AMER CHEMICAL SOC. - 1944-8244 .- 1944-8252. ; 12:6, s. 7557-7564
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Journal article (peer-reviewed)abstract
- The development of diblock copolymer (DBC) nanocomposite films containing magnetic nanoparticles (NPs) with diameters (D) over 20 nm is a challenging task. To host large iron oxide NPs (Fe3O4, D = 27 +/- 0.6 nm), an ultrahigh molecular weight (UHMW) linear DBC polystyrene-block-poly(methyl methacrylate) (PS-b-PMMA) is used as a template in the present work. Due to hydrogen bonding between the carboxylic acid ligands of the NPs and the ester groups in PMMA, the NPs show an affinity to the PMMA block. The localization of the NPs inside the DBC is investigated as a function of the NP concentration. At low NP concentrations, NPs are located preferentially at the interface between PS and PMMA domains to minimize the interfacial tension caused by the strong segregation strength of the UHMW DBC. At high NP concentrations (>= 10 wt %), chain-like NP aggregates (a head-to-tail orientation) are observed in the PMMA domains, resulting in a change of the morphology from sphere to ellipsoid for part of the PMMA domains. Magnetic properties of the hybrid films are probed via superconducting quantum interference device magnetometry. All hybrid films show ferrimagnetism and are promising for potential applications in magnetic data storage.
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| 5. |
- Cao, Wei, et al.
(author)
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Spray-Deposited Anisotropic Ferromagnetic Hybrid Polymer Films of PS-b-PMMA and Strontium Hexaferrite Magnetic Nanoplatelets
- 2021
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In: ACS Applied Materials and Interfaces. - : AMER CHEMICAL SOC. - 1944-8244 .- 1944-8252. ; 13:1, s. 1592-1602
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Journal article (peer-reviewed)abstract
- Spray deposition is a scalable and cost-effective technique for the fabrication of magnetic hybrid films containing diblock copolymers (DBCs) and magnetic nanoparticles. However, it is challenging to obtain spray-deposited anisotropic magnetic hybrid films without using external magnetic fields. In the present work, spray deposition is applied to prepare perpendicular anisotropic magnetic hybrid films by controlling the orientation of strontium hexaferrite nanoplatelets inside ultra-high-molecular-weight DBC polystyrene-block-poly(methyl methacrylate) (PS-b-PMMA) films. During spray deposition, the evolution of DBC morphology and the orientation of magnetic nanoplatelets are monitored with in situ grazing-incidence small-angle X-ray scattering (GISAXS). For reference, a pure DBC film without nanoplatelets is deposited with the same conditions. Solvent-controlled magnetic properties of the hybrid film are proven with solvent vapor annealing (SVA) applied to the final deposited magnetic films. Obvious changes in the DBC morphology and nanoplatelet localization are observed during SVA. The superconducting quantum interference device data show that ferromagnetic hybrid polymer films with high coercivity can be achieved via spray deposition. The hybrid films show a perpendicular magnetic anisotropy before SVA, which is strongly weakened after SVA. The spray-deposited hybrid films appear highly promising for potential applications in magnetic data storage and sensors.
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| 6. |
- Chen, Wei, et al.
(author)
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In situ Grazing-Incidence Small-Angle X-ray Scattering Observation of Gold Sputter Deposition on a PbS Quantum Dot Solid
- 2020
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In: ACS Applied Materials and Interfaces. - : NLM (Medline). - 1944-8244 .- 1944-8252. ; 12:41, s. 46942-46952
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Journal article (peer-reviewed)abstract
- For PbS quantum dot (QD)-based optoelectronic devices, gold is the most frequently used electrode material. In most device architectures, gold is in direct contact with the QD solid. To better understand the formation of the interface between gold and a close-packed QD layer at an early stage, in situ grazing-incidence small-angle X-ray scattering is used to observe the gold sputter deposition on a 1,2-ethanedithiol (EDT)-treated PbS QD solid. In the kinetics of gold layer growth, the forming and merging of small gold clusters (radius less than 1.6 nm) are observed at the early stages. The thereby formed medium gold clusters (radius between 1.9-2.4 nm) are influenced by the QDs' templating effect. Furthermore, simulations suggest that the medium gold clusters grow preferably along the QDs' boundaries rather than as a top coating of the QDs. When the thickness of the sputtered gold layer reaches 6.25 nm, larger gold clusters with a radius of 5.3 nm form. Simultaneously, a percolation layer with a thickness of 2.5 nm is established underneath the gold clusters. This fundamental understanding of the QD-gold interface formation will help to control the implementation of sputtered gold electrodes on close-packed QD solids in device manufacturing processes.
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| 7. |
- Gensch, Marc, et al.
(author)
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Correlating Nanostructure, Optical and Electronic Properties of Nanogranular Silver Layers during Polymer-Template-Assisted Sputter Deposition
- 2019
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In: ACS Applied Materials and Interfaces. - : AMER CHEMICAL SOC. - 1944-8244 .- 1944-8252. ; 11:32, s. 29416-29426
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Journal article (peer-reviewed)abstract
- Tailoring the optical and electronic properties of nanostructured polymer-metal composites demonstrates great potential for efficient fabrication of modern organic optical and electronic devices such as flexible sensors, transistors, diodes, or photovoltaics. Self-assembled polymer metal nanocomposites offer an excellent perspective for creating hierarchical nanostructures on macroscopic scales by simple bottom-up processes. We investigate the growth processes of nanogranular silver (Ag) layers on diblock copolymer thin film templates during sputter deposition. The Ag growth is strongly driven by self-assembly and selective wetting on the lamella structure of polystyrene-block-poly (methyl methacrylate). We correlate the emerging nanoscale morphologies with collective optical and electronic properties and quantify the difference in Ag growth on the corresponding homopolymer thin films. Thus, we are able to determine the influence of the respective polymer template and observe substrate effects on the Ag cluster percolation threshold, which affects the insulator-to-metal transition (IMT). Optical spectroscopy in the UV-vis regime reveals localized surface plasmon resonance for the metal polymer composite. Their maximum absorption is observed around the IMT due to the subsequent long-range electron conduction in percolated nanogranular Ag layers. Using X-ray photoelectron spectroscopy and Fourier-transform infrared spectroscopy, we identify the oxidation of Ag at the acrylate side chains as an essential influencing factor driving the selective wetting behavior in the early growth stages. The results of polymer-templated cluster growth are corroborated by atomic force microscopy and field emission scanning electron microscopy.
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| 8. |
- Gensch, Marc, et al.
(author)
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Selective Silver Nanocluster Metallization on Conjugated Diblock Copolymer Templates for Sensing and Photovoltaic Applications
- 2021
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In: ACS Applied Nano Materials. - : American Chemical Society (ACS). - 2574-0970. ; 4:4, s. 4245-4255
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Journal article (peer-reviewed)abstract
- Polymer-metal composite films with nanostructured metal and/or polymer interfaces show a significant perspective for optoelectronic applications, for example, as sensors or in organic photovoltaics (OPVs). The polymer components used in these devices are mostly nanostructured conductive polymers with conjugated pi-electron systems. Enhanced OPV's power conversion efficiencies or sensor sensitivity can be achieved by selective metal deposition on or into polymer templates. In this study, we exploit time-resolved grazing-incidence X-ray scattering to observe the metal-polymer interface formation and the cluster crystallite size in situ during silver (Ag) sputter deposition on a poly(3-hexylthiophene-2,5-diyl)-b-poly(methyl methacrylate) (PMMA-b-P3HT) template. We compare the arising nanoscale morphologies with electronic properties, determine Ag growth regimes, and quantify the selective Ag growth for the diblock copolymer (DBC) template using the corresponding homopolymer thin films (P3HT and PMMA) as a reference. Hence, we are able to describe the influence of the respective polymer blocks and substrate effects on the Ag cluster percolation: the percolation threshold is correlated with the insulator-to-metal transition measured in situ with resistance measurements during the sputter deposition. The Ag cluster percolation on PMMA-b-P3HT starts already on the network of the hexagonal P3HT domain before a complete metal film covers the polymer surface, which is complemented by microscopic measurements. In general, this study demonstrates a possible method for the selective Ag growth as a scaffold for electrode preparation in nanoelectronics and for energy harvesting applications.
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| 9. |
- Wang, Kun, et al.
(author)
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Comparison of UV Irradiation and Sintering on Mesoporous Spongelike ZnO lms Prepared from PS-b-P4VP Templated Sol-Gel Synthesis
- 2018
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In: ACS Applied Nano Materials. - : American Chemical Society (ACS). - 2574-0970. ; 1:12, s. 7139-7148
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Journal article (peer-reviewed)abstract
- Mesoporous ZnO films with large surface-area-to-volume ratio show great omise in multiple applications, among which solid-state dye-sensitized lar cells (ssDSSCs) have attracted great attention in the field of otovoltaics. An appropriate mesopore size in the nanostructured ZnO lms significantly plays an indispensable role in improving the device ficiency that resulted from an efficient penetration of dye molecules d solid hole transport material. In the present work, mesoporous ongelike ZnO films are prepared using sol-gel synthesis templated by a block copolymer polystyrene-block-poly(4-vinylpyridine). Two different mplate removal techniques, ultraviolet (UV) irradiation and gh-temperature sintering, are used to compare their respective impact the pore sizes of the final ZnO thin films. Both the surface rphology and the inner morphology show that mesopores obtained via UV radiation are smaller as compared to their sintered counterparts. reover, increasing the template-to-ZnO precursor ratio is found to rther enlarge present mesopores. Accordingly, a strong correlation tween the pore sizes of sol-gel synthesized ZnO films and photovoltaic rformance of fabricated ssDSSCs is demonstrated. In contrast with the vices fabricated from the UV-irradiated ZnO films, those obtained from ntered samples show >2 times higher efficiency.
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| 10. |
- Weindl, Christian L., et al.
(author)
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Effect of Solvent Vapor Annealing on Diblock Copolymer-Templated Mesoporous Si/Ge/C Thin Films : Implications for Li-Ion Batteries
- 2022
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In: ACS Applied Nano Materials. - : American Chemical Society (ACS). - 2574-0970. ; 5:5, s. 7278-7287
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Journal article (peer-reviewed)abstract
- Although amphiphilic diblock copolymer templating of inorganic materials such as TiO2 is already well investigated, sol-gel synthesis routines for porous silicon and germanium are relatively rare. Therefore, especially in the field of Li-ion batteries, novel synthesis routines with the possibility to tune the silicon and germanium ratio and the morphology in the nanometer regime are of high interest. Here, we demonstrate a synthesis method that allows a change of morphology and elemental composition with minimal effort. We evidence a morphological transformation in the nanometer regime with real space (scanning electron microscopy) and complementary reciprocal space analysis methods (grazing-incidence small-angle X-ray scattering). Although energy-dispersive X-ray spectroscopy (EDS) reveals a considerable amount of oxygen in the thin film, crystalline Ge in the bulk is detected with powder Xray diffraction (PXRD) and Raman spectroscopy. Due to the system's simplicity, chemical mass production options such as roll-to-roll or slot-die printing can also be considered high-yield methods compared to standard synthesis routines.
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