27 research outputs found
Solution-Printed Organic Semiconductor Blends Exhibiting Transport Properties on Par with Single Crystals
Solution-printed organic semiconductors have emerged in recent years as promising contenders for roll-to-roll manufacturing of electronic and optoelectronic circuits. The stringent performance requirements for organic thin-film transistors (OTFTs) in terms of carrier mobility, switching speed, turn-on voltage and uniformity over large areas require performance currently achieved by organic single-crystal devices, but these suffer from scale-up challenges. Here we present a new method based on blade coating of a blend of conjugated small molecules and amorphous insulating polymers to produce OTFTs with consistently excellent performance characteristics (carrier mobility as high as 6.7 cm2Vâ1sâ1, low threshold voltages of \u3c1V and low sub threshold swings \u3c0.5Vdecâ1). Our findings demonstrate that careful control over phase separation and crystallization can yield solution-printed polycrystalline organic semiconductor films with transport properties and other figures of merit on par with their single-crystal counterparts
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Combining text mining, in situ characterization, and ab initio calculations to rationalize BiFeO3 crystallization pathways
The combination of three highly complementary scientific domains is demonstrated to rationalize bismuth ferrite (BiFeO3 [BFO]) crystallization pathways: text mining to extract processing recipes from existing literature, in situ X-ray scattering to follow crystallization pathways of solution-processed thin films, and ab initio calculations to develop a comprehensive understanding of thin-film formation from thermodynamic principles. Multiferroic BFO is chosen as an example material of interest for technological applications to demonstrate and validate this combined approach. Thermodynamic modeling showed that the production of a short-lived intermediate bismutite phase (Bi2O2CO3) influences the energies of competing reactions forming BFO and Bi2Fe4O9, increasing the thermodynamic driving force toward the formation of BFO rather than Bi2Fe4O9 impurity phase over a large temperature window. The synergy between the scientific domains is exemplified through the rational guidelines developed for controlling high-quality and phase-pure material fabrication
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Text Mining the Literature to Inform Experiments and Rationalize Impurity Phase Formation for BiFeO3
We used data-driven methods to understand the formation of impurity phases in BiFeO3 thin-film synthesis through the sol-gel technique. Using a high-quality dataset of 331 synthesis procedures and outcomes extracted manually from 177 scientific articles, we trained decision tree models that reinforce important experimental heuristics for the avoidance of phase impurities but ultimately show limited predictive capability. We find that several important synthesis features, identified by our model, are often not reported in the literature. To test our ability to correctly impute missing synthesis parameters, we attempted to reproduce nine syntheses from the literature with varying degrees of âmissingnessâ. We demonstrate how a text-mined dataset can be made useful by informing new controlled experiments and forming a better understanding for impurity phase formation in this complex oxide system
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Mechanism of Additive-Assisted Room-Temperature Processing of Metal Halide Perovskite Thin Films.
Perovskite solar cells have received substantial attention due to their potential for low-cost photovoltaic devices on flexible or rigid substrates. Thiocyanate (SCN)-containing additives, such as MASCN (MA = methylammonium), have been shown to control perovskite film crystallization and the film microstructure to achieve effective room-temperature perovskite absorber processing. Nevertheless, the crystallization pathways and mechanisms of perovskite formation involved in MASCN additive processing are far from clear. Using in situ X-ray diffraction and photoluminescence, we investigate the crystallization pathways of MAPbI3 and reveal the mechanisms of additive-assisted perovskite formation during spin coating and subsequent N2 drying. We confirm that MASCN induces large precursor aggregates in solution and, during spin coating, promotes the formation of the perovskite phase with lower nucleation density and overall larger initial nuclei size, which forms upon reaching supersaturation in solution, in addition to intermediate solvent-complex phases. Finally, during the subsequent N2 drying, MASCN facilitates the dissociation of these precursor aggregates and the solvate phases, leading to further growth of the perovskite crystals. Our results show that the nature of the intermediate phases and their formation/dissociation kinetics determine the nucleation and growth of the perovskite phase, which subsequently impact the film microstructure. These findings provide mechanistic insights underlying room-temperature, additive-assisted perovskite processing and help guide further development of such facile room-temperature synthesis routes
Fullerene derivative induced morphology of bulk heterojunction blends: PIPCP:PC61BM.
The performance of organic solar cells (OSCs) depends crucially on the morphology in bulk heterojunctions (BHJs), including the degree of crystallinity of the polymer and the amount of each material phase: aggregated donor, aggregated acceptor, and molecular mixed donorâ:âacceptor phase. In this paper, we report the BHJ morphology of as-cast blend films incorporating the polymer PIPCP as the donor and [6,6]-phenyl-C61-butyric acid methyl ester (PC61BM) as the acceptor. Tracking the scattering intensity of PC61BM as a function of PC61BM concentration shows that PC61BM aggregates into donor-rich domains and there is little to no phase where the PC61BM and PIPCP are intimately mixed. We further find that on blending the scattering peak due to PIPCP ordering along the backbone increases with decreasing PIPCP fraction, which is attributed to improved ordering of PIPCP due to the presence of PC61BM. Our results suggest that the improved ordering of PIPCP along the backbone (consistent with an increased conjugation length) with blending contributes to the observed low open-circuit voltage energy loss
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Mixed Nanosphere Assemblies at a LiquidâLiquid Interface
The in-plane packing of gold (Au), polystyrene (PS), and silica (SiO2) spherical nanoparticle (NP) mixtures at a water-oil interface is investigated in situ by UV-vis reflection spectroscopy. All NPs are functionalized with carboxylic acid such that they strongly interact with amine-functionalized ligands dissolved in an immiscible oil phase at the fluid interface. This interaction markedly increases the binding energy of these nanoparticle surfactants (NPSs). The separation distance between the Au NPSs and Au surface coverage are measured by the maximum plasmonic wavelength (λmax) and integrated intensities as the assemblies saturate for different concentrations of non-plasmonic (PS/SiO2) NPs. As the PS/SiO2 content increases, the time to reach intimate Au NP contact also increases, resulting from their hindered mobility. λmax changes within the first few minutes of adsorption due to weak attractive inter-NP forces. Additionally, a sharper peak in the reflection spectrum at NP saturation reveals tighter Au NP packing for assemblies with intermediate non-plasmonic NP content. Grazing incidence small angle X-ray scattering (GISAXS) and scanning electron microscopy (SEM) measurements confirm a decrease in Au NP domain size for mixtures with larger non-plasmonic NP content. The results demonstrate a simple means to probe interfacial phase separation behavior using in situ spectroscopy as interfacial structures densify into jammed, phase-separated NP films