Publications
222 results found
Venkatram S, McCollum J, Stingelin N, et al., 2023, A close look at polymer degree of crystallinity versus polymer crystalline quality, Polymer International, Vol: 72, Pages: 855-860, ISSN: 0959-8103
In the broader polymer field, the term ‘crystallinity’ is often used rather loosely. However, increasingly, it becomes critical to clearly distinguish between degree of crystallinity, which provides the fractional amount of crystalline phase in a polymer, and the crystalline quality, which describes the perfection of the crystalline moieties that may form in a polymer. The reason is that these different structural features dictate important properties of plastic materials, including the mechanical properties of commodity polymers and the behavior of macromolecular ferroelectrics; they also determine which photophysical processes occur in semiconducting polymers. Hence, rigor needs to be applied when establishing structure/processing/property interrelations; and it should become a general practice that specific functions are clearly attributed to the degree of crystallinity, the crystalline quality or a combination of the two. In this perspective, in memoriam of Professor Dick Jones, a long-time member of IUPAC's Polymer Division, we discuss the challenges of identifying—and distinguishing between—these important structural characteristics when using commonly applied measuring techniques and/or theoretical approaches. This task is often elaborate, as small changes in the chemical nature of the polymer and/or processing conditions selected can have drastic effects on both the crystalline quality and the degree of crystallinity, an issue that combined with the general ambiguity of data obtained with methodologies used to characterize polymer structures, theoretically or experimentally based. © 2023 The Authors. Polymer International published by John Wiley & Sons Ltd on behalf of Society of Industrial Chemistry.
Stingelin N, Jurchescu OD, Wakayama Y, et al., 2023, Next-Generation Organic Semiconductors–Materials, Fundamentals, and Applications, Advanced Materials Interfaces, Vol: 10
Peng Z, Stingelin N, Ade H, et al., 2023, A materials physics perspective on structure–processing–function relations in blends of organic semiconductors, Nature Reviews Materials, Vol: 8, Pages: 439-455
During the past 30 years of research in organic electronics, the development of mechanistic understanding of important structure–processing–performance interrelationships has been slowly but steadily growing. Nevertheless, especially if blends are used in the active device layer, the development of new materials and device fabrication still predominantly relies on time-consuming trial-and-error procedures. In this Review, we demonstrate that well-established models, rooted in classical materials science and the thermodynamics of mixtures, can provide quantitative frameworks to guide material and process design. We provide, from a materials physics perspective, a concise and accessible overview on the relation between fundamental thermodynamic and kinetic principles relevant to (solution) processing, active layer morphology and stability of organic electronic devices based on blends by means of illustrative examples from organic photovoltaics. We aim to address a wide audience, including synthetic chemists, materials scientists, device engineers and beyond.
Khirbat A, Nahor O, Kantrow H, et al., 2023, Mission immiscible: overcoming the miscibility limit of semiconducting:ferroelectric polymer blends via vitrification, Journal of Materials Chemistry C, Vol: 11, Pages: 8300-8306, ISSN: 2050-7526
Blending offers a versatile processing platform to combine multiple properties in a given material system that may not be realized in one single component, or to induce co-operatively entirely new features. Polymers can, however, be challenging to blend due to their low tendency to mix, especially when processed from the melt. Here, we demonstrate that essentially the entire spectrum of phase morphologies, from basically fully intermixed to strongly phase-separated, can be induced reliably in blends produced from the archetypal polymer semiconductor, poly(3-hexyl thiophene), P3HT, and poly(vinylidene fluoride), PVDF, a polymer that can exhibit ferroelectric polymorphs, despite the intrinsically limited miscibility featured by P3HT and PVDF. We achieve this by manipulating chain entanglements in solution, which in turn dictates the molecular mobility of the two components (i.e., mass transport during solidification), and in extreme cases leads to pronounced vitrification in the solid state. Since partly- to well-intermixed systems can be produced when processed from a good solvent for both components, we conclude that entanglements form between P3HT and PVDF molecules, provided their molecular weight and concentration is sufficiently high. Hence, specific phase morphologies can be targeted towards broad materials discovery via the establishment of reliable interrelationships between structure, phase morphology, and properties.
Strang A, Quirós-Cordero V, Grégoire P, et al., 2023, Simple and Versatile Platforms for Manipulating Light with Matter: Strong Light-Matter Coupling in Fully Solution-Processed Optical Microcavities., Adv Mater
Planar microcavities with strong light-matter coupling, monolithically processed fully from solution, consisting of two polymer-based distributed Bragg reflectors (DBRs) comprising alternating layers of a high-refractive-index titanium oxide hydrate/poly(vinyl alcohol) hybrid material and a low-refractive-index fluorinated polymer are presented. The DBRs enclose a perylene diimide derivative (b-PDI-1) film positioned at the antinode of the optical mode. Strong light-matter coupling is achieved in these structures at the target excitation of the b-PDI-1. Indeed, the energy-dispersion relation (energy vs in-plane wavevector or output angle) in reflectance and the group delay of transmitted light in the microcavities show a clear anti-crossing-an energy gap between two distinct exciton-polariton dispersion branches. The agreement between classical electrodynamic simulations of the microcavity response and the experimental data demonstrates that the entire microcavity stack can be controllably produced as designed. Promisingly, the refractive index of the inorganic/organic hybrid layers used in the microcavity DBRs can be precisely manipulated between values of 1.50 to 2.10. Hence, microcavities with a wide spectral range of optical modes might be designed and produced with straightforward coating methodologies, enabling fine-tuning of the energy and lifetime of the microcavities' optical modes to harness strong light-matter coupling in a wide variety of solution processable active materials.
DiTullio BT, Kuang X, Österholm AM, et al., 2023, Additive manufacturing of polyaniline blends for lightweight structures with tunable conductivity, Journal of Materials Chemistry C, Vol: 11, Pages: 4404-4414
Printable feedstocks that can produce lightweight, robust, and ductile structures with tunable and switchable conductivity are of considerable interest for numerous application spaces. Combining the specific properties of commodity thermoplastics with the unique electrical and redox properties of conducting polymers (CPs) presents new opportunities for the field of printed (bio)electronics. Here, we report on the direct ink write (DIW) printing of ink formulations based on polyaniline-dinonylnaphthalene sulfonic acid (PANI-DNNSA), which has been synthesized in bulk quantities (∼400 g). DNNSA imparts solubility to PANI up to 50 mg mL−1, which allows the use of various additives to tune the rheological behavior of the inks without significantly compromising the electrical properties of the printed structures, which reach conductivities in the range of <10−7-100 S cm−1 as a function of ink formulation and post treatment used. Fumed silica (FS) and ultra-high molecular weight polystyrene (UHMW-PS) additives are leveraged to endow printability and shape retention to inks, as well as to compare the use of traditional rheological modifiers with commodity thermoplastics on CP feedstocks for tailored DIW printing. We show that the incorporation of UHMW-PS into these ink formulations is critical for obtaining high crack resistance in printed structures. This work serves as a guide for future ink designs of CPs with commodity thermoplastics and their subsequent DIW printing to yield conductive architectures and devices for various applications.
Brettmann B, Fraga MA, Gosecka M, et al., 2023, Introduction to Polymer Upcycling, Journal of Materials Chemistry A, Vol: 11, Pages: 5975-5977, ISSN: 2050-7488
Menezes NP, Nicolini T, Barker M, et al., 2023, Improved stability of organic electrochemical transistor performance with a low swelling mixed conducting polymer: a comparative study with PEDOT:PSS, Journal of Materials Chemistry C, ISSN: 2050-7526
Organic electrochemical transistors (OECTs) are bioelectronic devices that are capable of tracking biological events with extremely high sensitivity. Despite promising advances in terms of steady state performance, stable long-term electrochemical characteristics in complex environments need to be achieved in order for OECTs to open the market of biosensing applications. This work demonstrates the electrochemical performance stability of OECTs with a low swelling mixed conductor, poly[3-(6-hydroxy)hexylthiophene] (P3HHT), soaked in an electrolyte for up to 40 days, and the influence of the nature of the electrolyte on device performance.
Barker M, Nicolini T, Al Yaman Y, et al., 2022, Conjugated polymer blends for faster organic mixed conductors, MATERIALS HORIZONS, Vol: 10, Pages: 248-256, ISSN: 2051-6347
Augustyn V, Hatzell KB, Jeffries-EL M, et al., 2022, Introduction to the special collection in memoriam of Susan A. Odom (16 November 1980-18 April 2021), MATERIALS ADVANCES, Vol: 3, Pages: 7383-7383
Stingelin N, Rumbles G, 2022, In memoriam of Alasdair James Campbell, JOURNAL OF MATERIALS CHEMISTRY C, Vol: 10, Pages: 8894-8894, ISSN: 2050-7526
Gutierrez-Meza E, Malatesta R, Li H, et al., 2021, Frenkel biexcitons in hybrid HJ photophysical aggregates, SCIENCE ADVANCES, Vol: 7, ISSN: 2375-2548
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- Citations: 6
Vohlidal J, Graeff CFO, Hiorns RC, et al., 2021, Glossary of terms relating to electronic, photonic and magnetic properties of polymers (IUPAC Recommendations 2021), PURE AND APPLIED CHEMISTRY, Vol: 94, Pages: 15-69, ISSN: 0033-4545
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- Citations: 1
Yu L, Pavlica E, Li R, et al., 2021, Conjugated Polymer Mesocrystals with Structural and Optoelectronic Coherence and Anisotropy in Three Dimensions, ADVANCED MATERIALS, Vol: 34, ISSN: 0935-9648
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- Citations: 3
Luzio A, Martin J, Cheng CH, et al., 2021, Improving molecular alignment and charge percolation in semiconducting polymer films with highly localized electronic states through tailored thermal annealing, JOURNAL OF MATERIALS CHEMISTRY C, Vol: 9, Pages: 15848-15857, ISSN: 2050-7526
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- Citations: 5
Bachevillier S, Yuan H-K, Tetzner K, et al., 2021, Planar refractive index patterning through microcontact photo-thermal annealing of a printable organic/inorganic hybrid material, MATERIALS HORIZONS, Vol: 9, Pages: 411-416, ISSN: 2051-6347
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- Citations: 2
Matrone GM, Gutierrez-Meza E, Balzer AH, et al., 2021, The hole in the bucky: structure-property mapping of closed- vs. open-cage fullerene solar-cell blends via temperature/composition phase diagrams, JOURNAL OF MATERIALS CHEMISTRY C, Vol: 9, Pages: 16304-16312, ISSN: 2050-7526
Chen S, Haehnle B, Van der Laan X, et al., 2021, Understanding hierarchical spheres-in-grating assembly for bio-inspired colouration, MATERIALS HORIZONS, Vol: 8, Pages: 2230-2237, ISSN: 2051-6347
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- Citations: 6
Botiz I, Durbin MM, Stingelin N, 2021, Providing a Window into the Phase Behavior of Semiconducting Polymers, MACROMOLECULES, Vol: 54, Pages: 5304-5320, ISSN: 0024-9297
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- Citations: 4
Yu L, Portale G, Stingelin N, 2021, Solution-processing of semiconducting organic small molecules: what we have learnt from 5,11-bis(triethylsilylethynyl)anthradithiophene, JOURNAL OF MATERIALS CHEMISTRY C, Vol: 9, Pages: 10547-10556, ISSN: 2050-7526
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- Citations: 7
Marina S, Scaccabarozzi AD, Gutierrez-Fernandez E, et al., 2021, Polymorphism in Non-Fullerene Acceptors Based on Indacenodithienothiophene, ADVANCED FUNCTIONAL MATERIALS, Vol: 31, ISSN: 1616-301X
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- Citations: 18
Wade J, Higgins SG, Heutz S, et al., 2021, In memoriam Alasdair James Campbell (11 May 1961-27 February 2021), Journal of Materials Chemistry C, Vol: 9, Pages: 6100-6102, ISSN: 2050-7526
Nicolini T, Surgailis J, Savva A, et al., 2020, A Low-Swelling Polymeric Mixed Conductor Operating in Aqueous Electrolytes, ADVANCED MATERIALS, Vol: 33, ISSN: 0935-9648
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- Citations: 22
Scaccabarozzi AD, Basham J, Yu L, et al., 2020, High-density polyethylene-an inert additive with stabilizing effects on organic field-effect transistors, JOURNAL OF MATERIALS CHEMISTRY C, Vol: 8, Pages: 15406-15415, ISSN: 2050-7526
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- Citations: 12
Jones RG, Ober CK, Hayakawa T, et al., 2020, Terminology of polymers in advanced lithography (IUPAC Recommendations 2020), PURE AND APPLIED CHEMISTRY, Vol: 92, Pages: 1861-1891, ISSN: 0033-4545
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- Citations: 1
Thomas EM, Peterson KA, Balzer AH, et al., 2020, Effects of Counter-Ion Size on Delocalization of Carriers and Stability of Doped Semiconducting Polymers, ADVANCED ELECTRONIC MATERIALS, Vol: 6, ISSN: 2199-160X
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- Citations: 15
Marina S, Kaufmann NP, Karki A, et al., 2020, The Importance of Quantifying the Composition of the Amorphous Intermixed Phase in Organic Solar Cells, ADVANCED MATERIALS, Vol: 32, ISSN: 0935-9648
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- Citations: 13
Le Goupil F, Kallitsis K, Tence-Girault S, et al., 2020, Enhanced Electrocaloric Response of Vinylidene Fluoride-Based Polymers via One-Step Molecular Engineering, ADVANCED FUNCTIONAL MATERIALS, Vol: 31, ISSN: 1616-301X
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- Citations: 15
Sommerville PJW, Li Y, Dong BX, et al., 2020, Elucidating the Influence of Side-Chain Circular Distribution on the Crack Onset Strain and Hole Mobility of Near-Amorphous Indacenodithiophene Copolymers, MACROMOLECULES, Vol: 53, Pages: 7511-7518, ISSN: 0024-9297
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- Citations: 13
Levitsky A, Matrone GM, Khirbat A, et al., 2020, Toward Fast Screening of Organic Solar Cell Blends, ADVANCED SCIENCE, Vol: 7
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- Citations: 12
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