| 1. |
- Eckstein, Brian J., et al.
(författare)
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Processable High Electron Mobility pi-Copolymers via Mesoscale Backbone Conformational Ordering
- 2021
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Ingår i: Advanced Functional Materials. - : WILEY-V C H VERLAG GMBH. - 1616-301X .- 1616-3028. ; 31:15
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Tidskriftsartikel (refereegranskat)abstract
- The synthesis and experimental/theoretical characterization of a new series of electron-transporting copolymers based on the naphthalene bis(4,8-diamino-1,5-dicarboxyl)amide (NBA) building block are reported. Comonomers are designed to test the emergent effects of manipulating backbone torsional characteristics, and density functional theory (DFT) analysis reveals the key role of backbone conformation in optimizing electronic delocalization and transport. The NBA copolymer conformational and electronic properties are characterized using a broad array of molecular/macromolecular, thermal, optical, electrochemical, and charge transport techniques. All NBA copolymers exhibit strongly aggregated morphologies with significant nanoscale order. Copolymer charge transport properties are investigated in thin-film transistors and exhibit excellent electron mobilities ranging from 0.4 to 4.5 cm(2) V-1 s(-1). Importantly, the electron transport efficiency correlates with the film mesoscale order, which emerges from comonomer-dependent backbone planarity and extension. These results illuminate the key NBA building block structure-morphology-bulk property design relationships essential for processable, electronics-applicable high-performance polymeric semiconductors.
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| 2. |
- Wang, Gang, et al.
(författare)
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Aggregation control in natural brush-printed conjugated polymer films and implications for enhancing charge transport
- 2017
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Ingår i: Proceedings of the National Academy of Sciences of the United States of America. - : NATL ACAD SCIENCES. - 0027-8424 .- 1091-6490. ; 114:47, s. E10066-E10073
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Tidskriftsartikel (refereegranskat)abstract
- Shear-printing is a promising processing technique in organic electronics for microstructure/charge transport modification and large-area film fabrication. Nevertheless, the mechanism by which shear-printing can enhance charge transport is not well-understood. In this study, a printing method using natural brushes is adopted as an informative tool to realize direct aggregation control of conjugated polymers and to investigate the interplay between printing parameters, macromolecule backbone alignment and aggregation, and charge transport anisotropy in a conjugated polymer series differing in architecture and electronic structure. This series includes (i) semicrystalline hole-transporting P3HT, (ii) semicrystalline electron transporting N2200, (iii) low-crystallinity hole-transporting PBDTT-FTTE, and (iv) low-crystallinity conducting PEDOT:PSS. The (semi-)conducting films are characterized by a battery of morphology and microstructure analysis techniques and by charge transport measurements. We report that remarkably enhanced mobilities/conductivities, as high as 5.7x/3.9x, are achieved by controlled growth of nanofibril aggregates and by backbone alignment, with the adjusted R-2 (R-adj(2)) correlation between aggregation and charge transport as high as 95%. However, while shear-induced aggregation is important for enhancing charge transport, backbone alignment alone does not guarantee charge transport anisotropy. The correlations between efficient charge transport and aggregation are clearly shown, while mobility and degree of orientation are not always well-correlated. These observations provide insights into macroscopic charge transport mechanisms in conjugated polymers and suggest guidelines for optimization.
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| 3. |
- Wang, Gang, et al.
(författare)
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Mixed-flow design for microfluidic printing of two-component polymer semiconductor systems
- 2020
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Ingår i: Proceedings of the National Academy of Sciences of the United States of America. - : NATL ACAD SCIENCES. - 0027-8424 .- 1091-6490. ; 117:30, s. 17551-17557
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Tidskriftsartikel (refereegranskat)abstract
- The rational creation of two-component conjugated polymer sys-tems with high levels of phase purity in each component is challenging but crucial for realizing printed soft-matter electronics. Here, we report a mixed-flow microfluidic printing (MFMP) approach for two-component pi-polymer systems that significantly elevates phase purity in bulk-heterojunction solar cells and thin-film transistors. MFMP integrates laminar and extensional flows using a specially microstructured shear blade, designed with fluid flow simulation tools to tune the flow patterns and induce shear, stretch, and pushout effects. This optimizes polymer conformation and semi-conducting blend order as assessed by atomic force microscopy (AFM), transmission electron microscopy (TEM), grazing incidence wide-angle X-ray scattering (GIWAXS), resonant soft X-ray scattering (R-SoXS), photovoltaic response, and field effect mobility. For printed all-polymer (poly[(5,6-difluoro-2-octyl-2H-benzotriazole-4,7-diyl)-2,5-thiophenediyl[4,8-bis[5-(2-hexyldecyl)-2-thienyl]benzo[1,2-b:4,5-b ]dithiophene-2,6-diyl]-2,5-thiophenediyl]) [J51]:(poly{[N,N -bis(2-octyldodecyl) naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,5 -(2,2 -bithio-phene)}) [N2200]) solar cells, this approach enhances short-circuit currents and fill factors, with power conversion efficiency increasing from 5.20% for conventional blade coating to 7.80% for MFMP. Moreover, the performance of mixed polymer ambipolar [poly(3-hexylthiophene-2,5-diyl) (P3HT):N2200] and semiconducting:insulat-ing polymer unipolar (N2200:polystyrene) transistors is similarly enhanced, underscoring versatility for two-component pi-polymer systems. Mixed-flow designs offer modalities for achieving high-performance organic optoelectronics via innovative printing methodologies.
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