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Sökning: WFRF:(Müller Buschbaum Peter)

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1.
  • Bergendal, Erik, et al. (författare)
  • 3D texturing of the air-water interface by biomimetic self-assembly
  • 2020
  • Ingår i: Nanoscale Horizons. - : Royal Society of Chemistry. - 2055-6764 .- 2055-6756. ; 5:5, s. 839-846
  • Tidskriftsartikel (refereegranskat)abstract
    • A simple, insoluble monolayer of fatty acid is shown to induce 3D nanotexturing of the air-water interface. This advance has been achieved through the study of monolayers of a methyl-branched long chain fatty acid, analogous to those found on the surface of hair and wool, directly at the air-water interface. Specular neutron reflectometry combined with AFM probing of deposited monolayers shows pronounced 3D surface domains, which are absent for unbranched analogues and are attributed to hydrocarbon packing constraints. The resulting surface topographies of the water far exceed the height perturbation that can be explained by the presence of capillary waves of a free liquid surface. These have hitherto been considered the only source of perturbation of the flatness of a planar water interface under gravity in the absence of topographical features from the presence of extended, globular or particulate matter. This amounts to a paradigm shift in the study of interfacial films and opens the possibility of 3D texturing of the air-water interface.
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2.
  • Bergendal, Erik, et al. (författare)
  • 3D texturing of the air–water interface by biomimetic self-assembly
  • 2020
  • Ingår i: Nanoscale Horizons. - 2055-6764 .- 2055-6756. ; :5, s. 839-846
  • Tidskriftsartikel (refereegranskat)abstract
    • A simple, insoluble monolayer of fatty acid is shown to induce 3D nanotexturing of the air–water interface. This advance has been achieved through the study of monolayers of a methyl-branched long chain fatty acid, analogous to those found on the surface of hair and wool, directly at the air–water interface. Specular neutron reflectometry combined with AFM probing of deposited monolayers shows pronounced 3D surface domains, which are absent for unbranched analogues and are attributed to hydrocarbon packing constraints. The resulting surface topographies of the water far exceed the height perturbation that can be explained by the presence of capillary waves of a free liquid surface. These have hitherto been considered the only source of perturbation of the flatness of a planar water interface under gravity in the absence of topographical features from the presence of extended, globular or particulate matter. This amounts to a paradigm shift in the study of interfacial films and opens the possibility of 3D texturing of the air–water interface.
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3.
  • Betker, Marie, et al. (författare)
  • Sprayed Hybrid Cellulose Nanofibril-Silver Nanowire Transparent Electrodes for Organic Electronic Applications
  • 2023
  • Ingår i: ACS Applied Nano Materials. - : American Chemical Society (ACS). - 2574-0970. ; 6:14, s. 13677-13688
  • Tidskriftsartikel (refereegranskat)abstract
    • In times of climate change and resource scarcity, researchers are aiming to find sustainable alternatives to synthetic polymers for the fabrication of biodegradable, eco-friendly, and, at the same time, high-performance materials. Nanocomposites have the ability to combine several favorable properties of different materials in a single device. Here, we evaluate the suitability of two kinds of inks containing silver nanowires for the fast, facile, and industrial-relevant fabrication of two different types of cellulose-based silver nanowire electrodes via layer-by-layer spray deposition only. The Type I electrode has a layered structure, which is composed of a network of silver nanowires sprayed on top of a cellulose nanofibrils layer, while the Type II electrode consists of a homogeneous mixture of silver nanowires and cellulose nanofibrils. A correlation between the surface structure, conductivity, and transparency of both types of electrodes is established. We use the Haacke figure of merit for transparent electrode materials to demonstrate the favorable influence of cellulose nanofibrils in the spray ink by identifying Type II as the electrode with the lowest sheet resistance (minimum 5 ± 0.04 Ω/sq), while at the same time having a lower surface roughness and shorter fabrication time than Type I. Finally, we prove the mechanical stability of the Type II electrode by bending tests and its long-time stability under ambient conditions. The results demonstrate that the mixed spray ink of silver nanowires and cellulose nanofibrils is perfectly suitable for the fast fabrication of highly conductive organic nanoelectronics on an industrial scale.
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6.
  • Brett, Calvin, et al. (författare)
  • Nanocellulose-Assisted Thermally Induced Growth of Silver Nanoparticles for Optical Applications
  • 2021
  • Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 13:23, s. 27696-27704
  • Tidskriftsartikel (refereegranskat)abstract
    • Optically responsive materials are present in everyday life, from screens to sensors. However, fabricating large-area, fossil-free materials for functional biocompatible applications is still a challenge today. Nanocelluloses from various sources, such as wood, can provide biocompatibility and are emerging candidates for templating organic optoelectronics. Silver (Ag) in its nanoscale form shows excellent optical properties. Herein, we combine both materials using thin-film large-area spray-coating to study the fabrication of optical response applications. We characterize the Ag nanoparticle formation by X-ray scattering and UV-vis spectroscopy in situ during growth on the nanocellulose template. The morphology and optical properties of the nanocellulose film are compared to the rigid reference surface SiO2. Our results clearly show the potential to tailor the energy band gap of the resulting hybrid material.
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7.
  • Brett, Calvin, et al. (författare)
  • Water-Induced Structural Rearrangements on the Nanoscale in Ultrathin Nanocellulose Films
  • 2019
  • Ingår i: Macromolecules. - : American Chemical Society (ACS). - 0024-9297 .- 1520-5835. ; 52:12, s. 4721-4728
  • Tidskriftsartikel (refereegranskat)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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8.
  • Guo, Renjun, et al. (författare)
  • Degradation mechanisms of perovskite solar cells under vacuum and one atmosphere of nitrogen
  • 2021
  • Ingår i: Nature Energy. - : Springer Nature. - 2058-7546. ; 6:10, s. 977-
  • Tidskriftsartikel (refereegranskat)abstract
    • Extensive studies have focused on improving the operational stability of perovskite solar cells, but few have surveyed the fundamental degradation mechanisms. One aspect overlooked in earlier works is the effect of the atmosphere on device performance during operation. Here we investigate the degradation mechanisms of perovskite solar cells operated under vacuum and under a nitrogen atmosphere using synchrotron radiation-based operando grazing-incidence X-ray scattering methods. Unlike the observations described in previous reports, we find that light-induced phase segregation, lattice shrinkage and morphology deformation occur under vacuum. Under nitrogen, only lattice shrinkage appears during the operation of solar cells, resulting in better device stability. The different behaviour under nitrogen is attributed to a larger energy barrier for lattice distortion and phase segregation. Finally, we find that the migration of excessive PbI2 to the interface between the perovskite and the hole transport layer degrades the performance of devices under vacuum or under nitrogen. Understanding degradation mechanisms in perovskite solar cells is key to their development. Now, Guo et al. show a greater degradation of the perovskite structure and morphology for devices operated under vacuum than under nitrogen.
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9.
  • Harder, Constantin, et al. (författare)
  • Poly(sobrerol methacrylate) Colloidal Inks Sprayed onto Cellulose Nanofibril Thin Films for Anticounterfeiting Applications
  • 2024
  • Ingår i: ACS Applied Nano Materials. - : American Chemical Society (ACS). - 2574-0970. ; 7:9, s. 10840-10851
  • Tidskriftsartikel (refereegranskat)abstract
    • The colloidal layer formation on porous materials is a crucial step for printing and applying functional coatings, which can be used to fabricate anticounterfeiting paper. The deposition of colloidal layers and subsequent thermal treatment allows for modifying the hydrophilicity of the surface of a material. In the present work, wood-based colloidal inks are applied by spray deposition on spray-deposited porous cellulose nanofibrils (CNF) films. The surface modification by thermal annealing of the fabricated colloid-cellulose hybrid thin films is investigated in terms of layering and hydrophobicity. The polymer colloids in the inks are core-shell nanoparticles with different sizes and glass transition temperatures (T-g), thus enabling different and low thermal treatment temperatures. The ratio between the core polymers, poly(sobrerol methacrylate) (PSobMA), and poly(-butyl methacrylate) (PBMA) determines the T-g and hence allows for tailoring of the T-g. The layer formation of the colloidal inks on the porous CNF layer depends on the imbibition properties of the CNF layer which is determined by their morphology. The water adhesion of the CNF layer decreases due to the deposition of the colloids and thermal treatment except for the colloids with a size smaller than the void size of the porous CNF film. In this case, the colloids are imbibed into the CNF layer when T-g of the colloids is reached and the polymer chains transit in a mobile phase. Tailored aggregate and nanoscale-embedded hybrid structures are achieved depending on the colloid properties. The imbibition of these colloids into the porous CNF films is verified with grazing incidence small-angle X-ray scattering. This study shows a route for tuning the nanoscale structure and macroscopic physicochemical properties useful for anticounterfeiting paper.
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10.
  • Jiang, Xinyu, et al. (författare)
  • Film Formation Kinetics of Polymer Donor and Nonfullerene Acceptor Active Layers During Printing Out of 1,2,4-Trimethylbenzene in Ambient Conditions
  • 2023
  • Ingår i: Solar RRL. - : Wiley. - 2367-198X. ; 7:6
  • Tidskriftsartikel (refereegranskat)abstract
    • Slot-die coating is a promising upscaling fabrication method to promote commercialization in the field of organic solar cells. Herein, the nonfullerene active layer blend of a conjugated polymer PffBT4T-2OD and a small molecule acceptor EH-IDTBR, which is printed out of the nonhalogenated solvent 1,2,4-trimethylbenzene, is studied. The film formation kinetics of the active layer PffBT4T-2OD:EH-IDTBR is probed in terms of the temporal evolutions in morphology as well as molecular conformation and aggregation as revealed by in situ grazing-incidence small angle X-ray scattering and UV–vis spectroscopy during the film printing process. A five-regime mesoscale domain growth process is observed in the active layer from the liquid state to the final dry state. The solvent evaporation-induced domain growth is accompanied with molecular stacking in a distinct J-type aggregation of the acceptor and a slight H-type aggregation of the donor molecules. The printed active layers exhibit an edge-on dominated PffBT4T-2OD and a face-on dominated EH-IDTBR crystallite structure. Compared to the neat PffBT4T-2OD and EH-IDTBR films, in the active layer, the crystallite structure deviates slightly in lattice spacing.
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11.
  • Reb, Lennart K., et al. (författare)
  • Space‐ and Post‐Flight Characterizations of Perovskite and Organic Solar Cells
  • 2023
  • Ingår i: Solar RRL. - : Wiley. - 2367-198X. ; 7:9
  • Tidskriftsartikel (refereegranskat)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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12.
  • Reus, Manuel A., et al. (författare)
  • INSIGHT: in situ heuristic tool for the efficient reduction of grazing-incidence X-ray scattering data
  • 2024
  • Ingår i: Journal of applied crystallography. - : International Union of Crystallography (IUCr). - 0021-8898 .- 1600-5767. ; 57, s. 509-528
  • Tidskriftsartikel (refereegranskat)abstract
    • INSIGHT is a Python-based software tool for processing and reducing 2D grazing-incidence wide- and small-angle X-ray scattering (GIWAXS/GISAXS) data. It offers the geometric transformation of the 2D GIWAXS/GISAXS detector image to reciprocal space, including vectorized and parallelized pixelwise intensity correction calculations. An explicit focus on efficient data management and batch processing enables full control of large time-resolved synchrotron and laboratory data sets for a detailed analysis of kinetic GIWAXS/ GISAXS studies of thin films. It processes data acquired with arbitrarily rotated detectors and performs vertical, horizontal, azimuthal and radial cuts in reciprocal space. It further allows crystallographic indexing and GIWAXS pattern simulation, and provides various plotting and export functionalities. Customized scripting offers a one-step solution to reduce, process, analyze and export findings of large in situ and operando data sets.
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13.
  • Roth, Stephan V., et al. (författare)
  • Patterned Diblock co-polymer Thin Films as Templates for Advanced Anisotropic Metal Nanostructures
  • 2015
  • Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 7:23, s. 12470-12477
  • Tidskriftsartikel (refereegranskat)abstract
    • We demonstrate glancing-angle deposition of gold on a nanostructured diblock copolymer, namely polystytene-block-poly(methyl methacrylate) thin film. Exploiting the selective wetting of gold on the polystyrene block, we are able to fabricate directional hierarchical structures. We prove the asymmetric growth of the gold nanoparticles and are able to extract the different growth laws by in situ scattering methods. The optical anisotropy of these hierarchical hybrid materials is further probed by angular resolved spectroscopic methods. This approach enables us to tailor functional hierarchical layers in nanodevices, such as nanoantennae arrays, organic photovoltaics, and sensor electronics.
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14.
  • Sarkar, Kuhu, et al. (författare)
  • Monitoring structural dynamics of in situ spray-deposited zinc oxide films for application in dye-sensitized solar cells
  • 2014
  • Ingår i: ChemSusChem. - : Wiley-VCH Verlagsgesellschaft. - 1864-5631 .- 1864-564X. ; 7, s. 2140-2145
  • Tidskriftsartikel (refereegranskat)abstract
    • The spray-deposition technique is an effective and scalable method to deposit zinc oxide nanostructures, which are used as active layers for dye-sensitized solar cells (DSSCs) in the present study. The dynamics of structural evolution are studied with grazing incidence small-angle X-ray scattering during in situ spraying. Nanostructured films obtained through multiple spray shots provide suitable structural length scales, morphologies, and film thicknesses; this leads to reasonable performance in a DSSC with the highest short-circuit current density reported so far.
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15.
  • Tu, Suo, et al. (författare)
  • Improvement of the thermoelectric properties of PEDOT:PSS films via DMSO addition and DMSO/salt post-treatment resolved from a fundamental view
  • 2022
  • Ingår i: Chemical Engineering Journal. - : Elsevier BV. - 1385-8947 .- 1873-3212. ; 429
  • Tidskriftsartikel (refereegranskat)abstract
    • The combination of dimethyl sulfoxide (DMSO)-solvent doping and physical-chemical DMSO/salt de-doping in a sequence has been used to improve the thermoelectric (TE) properties of poly(3,4-ethylenedioxythiophene):poly (4-styrenesulfonate) (PEDOT:PSS) films. A high power factor of ca.105.2 mu W m(-1) K-2 has been achieved for the PEDOT:PSS film after post-treatment with 10 % sodium sulfite (Na2SO3) in the DMSO/salt mixture (v/v), outperforming sodium bicarbonate (NaHCO3). The initial DMSO-doping treatment induces a distinct phase separation by facilitating the aggregation of the PEDOT molecules. At the same time, the subsequent DMSO/salt dedoping post-treatment strengthens the selective removal of the surplus non-conductive PSS chains. Substantial alterations in the oxidation level, chain conformations, PEDOT crystallites and their preferential orientation are observed upon treatment on the molecular level. At the mesoscale level, the purification and densification of PEDOT-rich domains enable the realization of inter-grain coupling by the formation of the electronically well-percolated network. Thereby, both electrical conductivity and Seebeck coefficient are optimized.
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16.
  • Wang, Yilin, et al. (författare)
  • Control of the Crystallization and Phase Separation Kinetics in Sequential Blade-Coated Organic Solar Cells by Optimizing the Upper Layer Processing Solvent
  • 2023
  • Ingår i: Advanced Energy Materials. - : Wiley. - 1614-6832 .- 1614-6840. ; 13:7
  • Tidskriftsartikel (refereegranskat)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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17.
  • Weindl, Christian L., et al. (författare)
  • Effect of Solvent Vapor Annealing on Diblock Copolymer-Templated Mesoporous Si/Ge/C Thin Films : Implications for Li-Ion Batteries
  • 2022
  • Ingår i: ACS Applied Nano Materials. - : American Chemical Society (ACS). - 2574-0970. ; 5:5, s. 7278-7287
  • Tidskriftsartikel (refereegranskat)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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18.
  • Weindl, Christian L., et al. (författare)
  • Toluene‐Mediated Morphology Tuning of Diblock Copolymer‐Templated Porous Si/Ge/K/C Thin Films for Li‐Ion Batteries
  • 2023
  • Ingår i: Advanced Energy and Sustainability Research. - : Wiley. - 2699-9412 .- 2699-9412. ; 4:10
  • Tidskriftsartikel (refereegranskat)abstract
    • Amphiphilic diblock copolymer poly(styrene-b-ethylene oxide) templating in combination with sol–gel chemistry is utilized to synthesize porous mixed silicon/germanium/potassium/carbon (Si/Ge/K/C) thin films. As a Si/Ge source, the dissolvable Zintl phase K12Si12Ge5 is used. The toluene-mediated morphological changes in the porous mixed Si/Ge/K/C thin films are studied with scanning electron microscopy and grazing incidence small/wide-angle X-Ray scattering. A dichloromethane solvent vapor annealing step is applied to study the additional morphological transformation inside the films. Since Ge and Si are promising anode materials in Li-ion batteries, CR2032 half-cells are manufactured with the porous mixed Si/Ge/K/C thin films and characterized by cyclic voltammograms, cycling, and impedance spectroscopy.
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19.
  • Xiao, Tianxiao, et al. (författare)
  • Autonomous self-healing hybrid energy harvester based on the combination of triboelectric nanogenerator and quantum dot solar cell
  • 2024
  • Ingår i: Nano Energy. - : Elsevier BV. - 2211-2855 .- 2211-3282. ; 125
  • Tidskriftsartikel (refereegranskat)abstract
    • Realization of multi-source energy harvesting with one single device would maximize power output. Thus, it is emerging as a promising strategy towards renewable energy generation and has attracted worldwide attention in the past decades. Capable of capturing mechanical energy that is ubiquitous in the ambient environment, triboelectric nanogenerator (TENG) has been considered a novel yet effective source towards next-generation energy harvesting. In this work, a flexible hybrid energy harvester (HEH) is developed via the rational integration of autonomous self-healing TENG and high bending-stable lead sulfide quantum dot (PbS QD) solar cell, enabling independent electricity generation by two different mechanisms. The single-electrode mode TENG component with self-healing is realized by a polydimethylsiloxane/Triton X-100 (PDMS/TX100) mixture as the dielectric layer and the shared gold (Au) electrode, which generates 0.39 µA of output current (Iout), 24.6 V of output voltages (Vout), 15.4 nC of transfer charges (Qsc), and 7.80 mW m−2 of output power peak density. The thin-film solar cell component is based on a PbS QD layer as the light absorber with a planar structure fabricated under low-cost and compatible conditions, achieving 22.8 mA cm−2 of short-circuit current density (Jsc) and 4.92% of power conversion efficiency (PCE). As a proof of concept, an electronic watch is successfully powered by harnessing ambient mechanical and solar energy with a hybridized energy cell. This approach will offer more opportunities to construct a versatile platform towards remote monitoring and smart home systems.
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20.
  • Yin, Shanshan, et al. (författare)
  • Multidimensional Morphology Control for PS-b-P-4 VP Templated Mesoporous Iron (III) Oxide Thin Films
  • 2021
  • Ingår i: Advanced Materials Interfaces. - : Wiley. - 2196-7350. ; 8:14
  • Tidskriftsartikel (refereegranskat)abstract
    • Mesoporous alpha-Fe2O3 thin films with large area homogeneity demonstrate tremendous potential in multiple applications. In the present work, the synthesis of morphology-controlled alpha-Fe2O3 thin films is realized with polystyrene-block-poly(4-vinyl pyridine) (PS-b-P4VP) diblock copolymer assisted sol-gel chemistry. The solvent category (DMF and 1,4-dioxane) and polymer-to-FeCl3 ratio used for the solution preparation are systematically varied to tune the morphology of the thin films. For both solvents, DMF and 1,4-dioxane, nanocluster structures are obtained with low PS-b-P4VP concentration. When the concentration of PS-b-P4VP reaches the critical micelle concentration, spherical and wormlike porous structures are specifically formed in the DMF and 1,4-dioxane solvent system, respectively. Further increasing the polymer-to-FeCl3 ratios leads to the enlargement of the spherical pore sizes in the DMF system, whereas the center-to-center distances of the wormlike structures in the 1,4-dioxane system decrease. Moreover, DMF/1,4-dioxane solvent mixtures with different volume ratios are applied for the sol-gel solution preparation to gain more insight into how the solvent selectivity affects the thin film morphology. By adjusting the preferential affinity of the solvent mixture to the polymer blocks, a spherical to wormlike pore shape transition is observed with a critical Delta chi value of around 0.77.
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22.
  • Zou, Yuqin, et al. (författare)
  • Ionic liquids tailoring crystal orientation and electronic properties for stable perovskite solar cells
  • 2023
  • Ingår i: Nano Energy. - : Elsevier BV. - 2211-2855 .- 2211-3282. ; 112, s. 108449-108449
  • Tidskriftsartikel (refereegranskat)abstract
    • The crystallization behavior of perovskite films has a profound influence on the resulting defect densities, charge carrier dynamics and photovoltaic performance. Herein, we introduce ionic liquids into the perovskite component to tailor the crystal growth of perovskite films from a disordered to a preferential corner-up orientation and accordingly increase the charge carrier mobility to accelerate electron transport and extraction. Using time-resolved measurements, we probe the charge carrier generation, transport and recombination behavior in these films and related devices. We find the ionic liquid-containing samples exhibit lower defects, faster charge carrier transport and suppressed non-radiative recombination, contributing to higher efficiency and fill factor. Via operando grazing-incidence small- and wide-angle X-ray scattering measurements, we observe a light-induced lattice compression and grain fragmentation in the control devices, whereas the ionic liquid-containing devices exhibit a slight light-induced crystal reconstitution and stronger tolerance against illumination. Under ambient conditions, the non-encapsulated device with the pyrrolidinium-based ionic compound (Pyr14BF4) maintains 97% of its initial efficiency after 4368 h.
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