| 1. |
- Akinsinde, Lewis O., et al.
(author)
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Surface characterization and resistance changes of silver-nanowire networks upon atmospheric plasma treatment
- 2021
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In: Applied Surface Science. - : Elsevier BV. - 0169-4332 .- 1873-5584. ; 550
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Journal article (peer-reviewed)abstract
- Highly conductive silver-nanowire (Ag-NW) networks are used in composite materials as conductive channels. Their resistance tuning can be accomplished by changing the Ag-NW concentration, and, therefore, changing the network structure. In this study, an alternative pathway to resistance engineering of conductive Ag-NW networks by local atmospheric plasma treatment is employed. The corresponding changes in nanowire network morphology and crystallinity as a function of plasma etching time are investigated by time-resolved grazingincidence X-ray scattering, field-effect scanning electron microscopy, and X-ray photoelectron spectroscopy. Three characteristic etching phases are identified. The first two phases enable the controlled engineering of the electrical properties with different rates of resistance change, which results from changes in nanowire shape, network morphology, and different oxidation rates. Phase III is characterized by pronounced fragmentation and destruction of the Ag-NW networks. These results show the feasibility of atmospheric plasma treatments to tune the local electrical properties of conductive Ag-NW networks. Furthermore, we present a physical Monte Carlo model explaining the electrical network properties as a function of plasma etching time based on the network connectivity and a constant plasma etching rate of 570 ng s-1 cm-2.
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| 2. |
- 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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| 3. |
- Chen, Qing, et al.
(author)
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Layer-by-Layer Spray-Coating of Cellulose Nanofibrils and Silver Nanoparticles for Hydrophilic Interfaces
- 2021
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In: ACS Applied Nano Materials. - : American Chemical Society (ACS). - 2574-0970. ; 4:1, s. 503-513
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Journal article (peer-reviewed)abstract
- Silver nanoparticles (AgNPs) and AgNP-based composite materials have attracted growing interest due to their structure-dependent optical, electrical, catalytic, and stimuli-responsive properties. For practical applications, polymeric materials are often combined with AgNPs to provide flexibility and offer a scaffold for homogenous distribution of the AgNPs. However, the control over the assembly process of AgNPs on polymeric substrates remains a big challenge. Herein, we report the fabrication of AgNP/cellulose nanofibril (CNF) thin films via layer-by-layer (LBL) spray-coating. The morphology and self-assembly of AgNPs with increasing number of spray cycles are characterized by atomic force microscopy (AFM), grazing-incidence small-angle X-ray scattering (GISAXS), and grazing-incidence wide-angle X-ray scattering (GIWAXS). We deduce that an individual AgNP (radius = 15 +/- 3 nm) is composed of multiple nanocrystallites (diameter = 2.4 +/- 0.9 nm). Our results suggest that AgNPs are assembled into large agglomerates on SiO2 substrates during spray-coating, which is disadvantageous for AgNP functionalization. However, the incorporation of CNF substrates contributes to a more uniform distribution of AgNP agglomerates and individual AgNPs by its network structure and by absorbing the partially dissolved AgNP agglomerates. Furthermore, we demonstrate that the spray-coating of the AgNP/CNF mixture results in similar topography and agglomeration patterns of AgNPs compared to depositing AgNPs onto a precoated CNF thin film. Contact-angle measurements and UV/vis spectroscopy suggest that the deposition of AgNPs onto or within CNFs could increase the hydrophilicity of AgNP-containing surfaces and the localized surface plasmon resonance (LSPR) intensity of AgNP compared to AgNPs sprayed on SiO(2 )substrates, suggesting their potential applications in antifouling coatings or label-free biosensors. Thereby, our approach provides a platform for a facile and scalable production of AgNP/CNF films with a low agglomeration rate by two different methods as follows: (1) multistep layer-by-layer (LBL) spray-coating and (2) direct spray-coating of the AgNP/CNF mixture. We also demonstrate the ability of CNFs as a flexible framework for directing the uniform assembly of AgNPs with tailorable wettability and plasmonic properties.
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| 4. |
- Chumakova, Aleksandra, et al.
(author)
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Exploring the Crystalline Structure of Gold Mesocrystals Using X-ray Diffraction
- 2023
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In: Crystals. - : MDPI AG. - 2073-4352. ; 13:8
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Journal article (peer-reviewed)abstract
- Mesocrystals are a class of nanostructured material where individual nanocrystals are arranged in a distinct crystallographic orientation. The multiple-length-scale order in such materials plays an essential role in the emergent physical and chemical phenomena. Our work studies the structure of a faceted mesocrystal composed of polystyrene-functionalized single crystalline gold nanoparticles using complementary ultrasmall- and wide-angle X-ray scattering (USAXS and WAXS) with electron microscopy. The results of the data analysis shed some light on the details of the microscopic structure of mesocrystals and their structuration principle.
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| 5. |
- Coupette, Fabian, et al.
(author)
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Percolation of rigid fractal carbon black aggregates
- 2021
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In: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 155:12
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Journal article (peer-reviewed)abstract
- We examine network formation and percolation of carbon black by means of Monte Carlo simulations and experiments. In the simulation, we model carbon black by rigid aggregates of impenetrable spheres, which we obtain by diffusion-limited aggregation. To determine the input parameters for the simulation, we experimentally characterize the micro-structure and size distribution of carbon black aggregates. We then simulate suspensions of aggregates and determine the percolation threshold as a function of the aggregate size distribution. We observe a quasi-universal relation between the percolation threshold and a weighted average radius of gyration of the aggregate ensemble. Higher order moments of the size distribution do not have an effect on the percolation threshold. We conclude further that the concentration of large carbon black aggregates has a stronger influence on the percolation threshold than the concentration of small aggregates. In the experiment, we disperse the carbon black in a polymer matrix and measure the conductivity of the composite. We successfully test the hypotheses drawn from simulation by comparing composites prepared with the same type of carbon black before and after ball milling, i.e., on changing only the distribution of aggregate sizes in the composites.& nbsp;
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| 6. |
- Jatav, Hemant, et al.
(author)
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Investigating the thermal stability of ultra-small Ag, Au and AuAg alloy nanoparticles embedded in a silica matrix
- 2023
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In: Nanoscale. - : Royal Society of Chemistry (RSC). - 2040-3364 .- 2040-3372. ; 15:28, s. 12025-12037
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Journal article (peer-reviewed)abstract
- Thermal growth kinetics of embedded bimetallic (AuAg/SiO2) nanoparticles are explored and compared with their monometallic (Au/SiO2 and Ag/SiO2) counterparts, as their practical applicability demands stability and uniformity. The plasmonic properties of these nanoparticles (NPs) significantly improve when their size falls in the ultra-small region (diameter < 10 nm), owing to their large active surface area. Interestingly, the bimetallic NPs exhibit better optical properties and structural stability as compared to their monometallic counterparts. This calls for a thorough understanding of the nucleation and temperature-dependent growth to ensure size stability against thermal coarsening that most bimetallic NPs completely lack. Herein, the atom beam sputtered AuAg NPs are systematically analysed over a wide range of annealing temperatures (ATs), and the results are compared with those of Au and Ag NPs. The X-ray photoelectron spectroscopy spectra and other experimental results confirm the formation of AuAg alloy NPs inside the silica matrix. Furthermore, techniques like transmission electron microscopy and grazing-incidence small-/wide-angle X-ray scattering were used to explore the temperature-dependent structural and morphological stability of the NPs. Our results show that the deposited AuAg NPs retain their spherical shape and remain as an alloy for the entire range of ATs. When the AT increases from 25 °C to 800 °C, the size of the NPs also increases from 3.5 to 4.8 nm; beyond that, their size grows substantially to 13.6 nm at 900 °C. We observed that the NPs remain in the ultra-small size range (∼5 nm) until an AT of 800 °C. Beyond that Ostwald ripening is ascribed to be the major cause of particle growth, resulting in an active surface area loss. Based on the outcomes, a three-step nucleation and growth mechanism is proposed.
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| 7. |
- Lin, Baojun, et al.
(author)
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Balancing the pre-aggregation and crystallization kinetics enables high efficiency slot-die coated organic solar cells with reduced non-radiative recombination losses
- 2020
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In: Energy & Environmental Science. - : Royal Society of Chemistry (RSC). - 1754-5692 .- 1754-5706. ; 13:8, s. 2467-2479
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Journal article (peer-reviewed)abstract
- Slot-die coating being compatible with the roll-to-roll technique has been regarded as a promising tool for upscaling the manufacturing of organic solar cells (OSCs). However, there has been a significant gap between the efficiencies of the state-of-the-art spin-coated devices and the scalable processed devices. The active layer morphology is crucial to achieve high efficiency in OSCs, which depends on the conditions of film fabrication. To figure out and optimize the slot-die coating process, a deeper understanding of the film formation kinetics is important. Herein, in situ measurements of the slot-die coating process based on the PM7:IT4F system are demonstrated to illustrate the aggregation and crystallization evolution at various die temperatures and substrate temperatures. OSCs with a high power conversion efficiency of 13.2% are achieved at 60 degrees C die temperature/60 degrees C substrate temperature due to the improved exciton dissociation, charge transport and suppressed non-radiative charge recombination. The optimized morphology is attributed to the balanced polymer pre-aggregation and small molecule crystallization kinetics. The unsuitable die temperature leads to overlarge phase separation and consequently inefficient exciton dissociation while the improper substrate temperature results in weak crystallization and the following shrunken carrier lifetime with strong non-radiative combination. This work provides fundamental understanding on the correlations among processing methodology, solution pre-aggregation, morphology formation kinetics, device physics and device performance and affords guidance for device optimization in scalable manufacturing.
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| 8. |
- Reb, Lennart K., et al.
(author)
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Space‐ and Post‐Flight Characterizations of Perovskite and Organic Solar Cells
- 2023
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In: Solar RRL. - : Wiley. - 2367-198X. ; 7:9
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Journal article (peer-reviewed)abstract
- Perovskite and organic solar cells are promising for space applications for enabling higher specific powers or alternative deployment systems. However, terrestrial tests can only mimic space conditions to a certain extent. Herein, a detailed analysis of irradiation-dependent photovoltaic parameters of perovskite and organic solar cells exposed to space conditions during a suborbital flight is presented. In orbital altitudes, perovskite and organic solar cells reach power-conversion efficiencies of more than 13% and 6%, respectively. Based on postflight grazing-incidence small-angle and wide-angle X-ray scattering, the active layer morphology and crystalline structure of the returned space solar cells are studied and compared to those of reference solar cells that stayed in an inert atmosphere. Minor changes in the active layer morphology are induced by the sole transport, without causing significant performance loss. For the space solar cells, morphological changes are attributed to the flight experiment that includes rocket launch, spaceflight, and reentry, as well as short-terrestrial environment exposure before and after launch. In contrast, no significant changes to the crystalline phase are observed. The notable performance during flight and high active layer stability, especially of perovskite solar cells, are promising results for further steps toward an orbital demonstration.
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| 9. |
- Ribca, Iuliana, 1993-, et al.
(author)
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Exploring the Effects of Different Cross-Linkers on Lignin-Based Thermoset Properties and Morphologies
- 2021
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In: ACS Sustainable Chemistry and Engineering. - : American Chemical Society (ACS). - 2168-0485. ; 9:4, s. 1692-1702
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Journal article (peer-reviewed)abstract
- The search for sustainable material solutions has put lignin as one of the prime candidates for aromatic building blocks in macromolecular materials. The present study aimed to demonstrate how lignin-based thermoset resins can be utilized in combination with different cross-linkers. Kraft lignin was used to produce thermosets with tunable mechanical and morphological properties. The lignin-based thermosets were obtained via a thermally induced thiol–ene reaction. The first part of this work was focused on Kraft lignin solvent fractionation and chemical modification of the ethanol soluble fraction. Chemical analysis indicated that the allylation process was selective toward phenolic hydroxyl groups. SAXS and SEM studies demonstrated that solvent fractionation and allylation processes affected the molecular and nanoscale morphological characteristics of lignin. The second part’s focus was on how the properties of thermosets can be tuned by using three different cross-linkers. The dynamic mechanical and morphological properties of three different thermosets were investigated via DMA, SAXS, and WAXS techniques. The three different thermosets exhibit similar molecular morphology but different storage modulus and glass transition temperature. In this work, it was shown that despite lignin’s heterogeneity it was possible to produce thermosetting materials with tunable properties.
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| 10. |
- Wang, Yilin, et al.
(author)
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Control of the Crystallization and Phase Separation Kinetics in Sequential Blade-Coated Organic Solar Cells by Optimizing the Upper Layer Processing Solvent
- 2023
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In: Advanced Energy Materials. - : Wiley. - 1614-6832 .- 1614-6840. ; 13:7
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Journal article (peer-reviewed)abstract
- Sequential deposition of the active layer in organic solar cells (OSCs) is favorable to circumvent the existing drawbacks associated with controlling the microstructure in bulk-heterojunction (BHJ) device fabrication. However, how the processing solvents impact on the morphology during sequential deposition processes is still poorly understood. Herein, high-efficiency OSCs are fabricated by a sequential blade coating (SBC) through optimization of the morphology evolution process induced by processing solvents. It is demonstrated that the device performance is highly dependent on the processing solvent of the upper layer. In situ morphology characterizations reveal that an obvious liquid–solid phase separation can be identified during the chlorobenzene processing of the D18 layer, corresponding to larger phase separation. During chloroform (CF) processing of the D18 layer, a proper aggregation rate of Y6 and favorable intermixing of lower and upper layers results in the enhanced crystallinity of the acceptor. This facilitates efficient exciton dissociation and charge transport with an inhibited charge recombination in the D18/CF-based devices, contributing to a superior performance of 17.23%. These results highlight the importance of the processing solvent for the upper layer in the SBC strategy and suggest the great potential of achieving optimized morphology and high-efficiency OSCs using the SBC strategy.
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| 11. |
- Zhai, Chenyang, et al.
(author)
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Surface Etching of Polymeric Semiconductor Films Improves Environmental Stability of Transistors
- 2021
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In: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 33:7, s. 2673-2682
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Journal article (peer-reviewed)abstract
- Solution-processed polymeric semiconductor films are attracting wide interest for applications in flexible electronics, wherein environmental stability is still a big obstacle. In many polymeric thin-film electronic devices, vertical phase separation has been observed, which leads to film depth dependences of electronic properties. Here, a soft plasma-assisted surface etching method to improve the environmental stability and maintain the electronic properties of organic field-effect transistors (OFETs) is proposed, by which the unwanted thin-film surface (exposed to air) is selectively taken away upon soft plasma etching, and the layer beneath the surface (subsurface) is preserved without any damage to the subsurface's structure or electronic function. Investigation of frequently used polymeric semiconductors poly(3-hexylthiophene) and poly[4-(4,4-dihexadecyl-4H-cyclopenta[1,2-b:5,4b']dithiophen-2-yl)-alt [1,2,5]thiadiazolo[3,4-c]pyridine] shows that the crystallinity of the surface layer is higher than that of the subsurface layer. However, for p-type polymeric semiconductors, higher crystallinity usually leads to a lower ionization energy and higher doping concentration during exposure to air and thus a higher background conductivity, deteriorating the switching-off capability of the organic field-effect transistors (OFETs). Therefore, by removing this surface layer, the lifetime of OFETs in air is effectively increased by over 50%.
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