Spark Discharge Doping—Achieving Unprecedented Control over Aggregate Fraction and Backbone Ordering in Poly(3‐hexylthiophene) Solutions

Eller, Fabian; Wenzel, Felix A.; Hildner, Richard; Havenith, Remco W. A.; Herzig, Eva M.

doi:10.1002/smll.202207537

Cited by 3 publications

(9 citation statements)

References 66 publications

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“…Aside from producing well-ordered, high-performance, OMIECs through heteroatom substitution, learning from these heteroatom effects provides rational structural targets for high performing, ion-efficient, and low-temperature OMIECs and OECTs. Beyond heteroatom substitution (which brings with it issues of material and device stability), these microstructures that benefit mixed conduction are likely achievable through alternate means, such as solution preaggregation, 66 film postprocessing, 47 or film/fiber strain alignment. 67 Thus, this study both maps a new route for microstructural control of OMIECs but also provides the direction for future synthetic, structural, and processing studies.…”

Section: ■ Conclusionmentioning

confidence: 99%

Enhancement of Conjugated Polymer Microstructure and Mixed-Conducting Properties via Chalcogenophene Heteroatom Substitution

Paulsen,

Meli,

Moser

et al. 2024

Chem. Mater.

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Heteroatom substitution is a powerful tool to tune the intra-and intermolecular structure of conjugated polymers as well as their resulting optoelectronic and electrochemical properties. A series of oligoethylene glycol bithiophene chalcogenophene polymers (p(g3T2-X)) with systematically varied furan, thiophene, selenophene, and tellurophene comonomers have been synthesized for mixed ionic-electronic conducting applications. Their microstructures have been thoroughly characterized ex situ and in situ with X-ray scattering, and their mixed conducting properties have been probed in electrochemical transistor testbeds. Chalcogenophene heteroatom choice was found to clearly dictate the polymer microstructure (crystallite dimensionality and orientation) and tune mixed conducting properties. Proceeding down Group 16, from O to Se systematically directed the molecular ordering of 2D polymer crystallites from face-on (O) to mixed (S) to edge-on (Se) orientations, with Te driving the polymer to form well-oriented edge-on 3D crystallites. Heteroatom dictated crystallite quality, and orientation tuned relative ionic transport by 2 orders of magnitude. Hole mobility (μ hole ) and mixed conducting figure of merit (μC*) were each tuned over an order of magnitude depending on heteroatom choice, with the Te-containing polymer reaching μ hole = 3.60 cm 2 V −1 s −1 and μC* = 483 F cm −1 V −1 s −1 , due to improved molecular ordering. Insights from this polymer series highlight target microstructures for enhanced mixed conduction in future conjugated polymers.

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Section: ■ Conclusionmentioning

confidence: 99%

Enhancement of Conjugated Polymer Microstructure and Mixed-Conducting Properties via Chalcogenophene Heteroatom Substitution

Paulsen,

Meli,

Moser

et al. 2024

Chem. Mater.

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“…CID Treatment: Since this work is interested to exploit highly ordered aggregates, chloroform as solvent was chosen at a temperature of 20 °C with a voltage of 300 V for charging the capacitor, which yielded the highest aggregate quality in this extensive previous study. [21] The untreated P3HT solutions were prepared by dissolving P3HT in chloroform at 50 °C for 20 min. Prior to the CID treatment, the solutions were kept for 15 min at 20 °C to allow for proper equilibration.…”

Section: Methodsmentioning

confidence: 99%

“…This procedure of charging the capacitor, connecting, and approaching the tungsten wires was repeated until the desired number of CID treatment steps was achieved. [21] Sample Preparation: The glass and silicon substrates were cut to the desired size and then thoroughly cleaned by sonication in Alconox, VEwater, and isopropanol for 10 min each. To ensure a comparable surface all samples were spin-coated with sonicated PEDOT:PSS at 3000 rpm.…”

Section: Methodsmentioning

confidence: 99%

“…Moreover, the solvent as well as concentration, and especially the temperature during treatment play an important role. [21] We want to investigate the influence of the CID treatment on the film formation of neat P3HT and especially on blends with Y12, a highly miscible Y-series NFA with alkyl chains identical to ZY-4Cl. To control the aggregate fraction in the solution prior to casting the films, we varied the number of CID steps.…”

Section: Introductionmentioning

confidence: 99%

“…[ 11,18–20 ] Thus, chemical modification of NFAs is one possibility to achieve phase separation. Here we demonstrate that applying a new technique called current‐induced doping (CID) [ 21 ] to obtain high‐quality P3HT aggregates in solution can improve the P3HT aggregation in dried thin films with and without a second component present and hence causing an effective phase separation in an otherwise miscible material system.…”

Section: Introductionmentioning

confidence: 99%

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Tackling P3HT:Y‐Series Miscibility Through Advanced Processing for Tunable Aggregation

Eller,

McNeill,

Herzig

2024

Advanced Energy Materials

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Polymer and small molecule blend thin films are of strong interest for organic electronics and particularly organic solar cells. The high miscibility in blends of ordinary P3HT and state‐of‐the‐art Y‐series non‐fullerene acceptors (NFAs) suppresses phase separation and aggregation challenging successful charge separation and transport. In this recent work, current‐induced doping (CID) is introduced, a method to precisely control the aggregation of Poly(3‐hexylthiophene) (P3HT) grazing incidence wide angle X‐ray scattering in solution. The highly ordered pre‐aggregation in solution is used here to control the P3HT aggregation in neat films and blends with Y12 (BTP‐4F‐12). This results in a 25‐fold increase in hole mobility in P3HT organic field‐effect transistor (OFET) devices and tunability of the P3HT aggregate quality in the presence of Y12 over large ranges. At the same time, particularly the Y12 long‐range ordering is heavily suppressed by increasing P3HT aggregation. However, solvent vapor annealing (SVA) leads to an extraordinarily high Y12 ordering, changes in the crystal orientation of Y12, and a further improvement of P3HT aggregation. A broad range of different degrees of aggregation of both materials can therefore be obtained in the final thin films solely by changing processing parameters without changing the composition of the material system.

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Facilitating Absorption Spectroscopy of Strongly Absorbing Fluids: A High-Throughput Approach

Eller,

Herzig

2024

J. Phys. Chem. A

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Measuring absorption spectra of strongly absorbing solutions is usually only possible by diluting the solution. However, the absorption spectra can be heavily influenced by concentrationdependent interactions, so dilution leads to misleading results. To enable reliable absorption measurements of concentrated solutions, we introduce in this work thinning fluid film spectroscopy (TFFS), a simple and highly automatable method. We present three exemplary measurement modes of TFFS suitable for many different applications and validate the TFFS measurements with control data obtained in specialized, low optical path length cuvettes. Additionally, we compare the suitability of the different measurement modes over a broad concentration range and demonstrate the automation possibilities with a spectroscopy robot. Beyond this automated approach for highly efficient and high-throughput lab work, we also show the possibility of direct integration into production systems with an in-line setup, which can be incorporated into a variety of pipe systems. The TFFS method is not limited to samples from material science but can be transferred to a broad variety of research and industry fields, including proteins, food, and pharmaceuticals or also agriculture and forensics.

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Spark Discharge Doping—Achieving Unprecedented Control over Aggregate Fraction and Backbone Ordering in Poly(3‐hexylthiophene) Solutions

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Cited by 3 publications

References 66 publications

Enhancement of Conjugated Polymer Microstructure and Mixed-Conducting Properties via Chalcogenophene Heteroatom Substitution

Enhancement of Conjugated Polymer Microstructure and Mixed-Conducting Properties via Chalcogenophene Heteroatom Substitution

Tackling P3HT:Y‐Series Miscibility Through Advanced Processing for Tunable Aggregation

Facilitating Absorption Spectroscopy of Strongly Absorbing Fluids: A High-Throughput Approach

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