Liyang Yu

Thermoelectric plastics: from design to synthesis, processing and structure–property relationships

Thermoelectric plastics are a class of polymer-based materials that combine the ability to directly convert heat to electricity, and vice versa, with ease of processing.

Additive-assisted supramolecular manipulation of polymer:fullerene blend phase morphologies and its influence on photophysical processes

It is well known that even small variations in the solid-state microstructure of polymer:fullerene bulk heterojunctions can drastically change their organic solar cell device performance. We employ pBTTT:PC61BM as a model system and manipulate co-crystal formation of 1 : 1 (by weight) blends with the assistance of fatty acid methyl esters as additives. This allows us to evaluate the role of the intermixed phase in such binary blends through manipulation of their phase morphology—from fully intercalated to partially and predominantly non-intercalated systems—and its effect on the exciton- and carrier- dynamics and the efficiency of charge collection, with relevance for future device design and manufacturing.

Hybrid Perovskite Thin‐Film Photovoltaics: In Situ Diagnostics and Importance of the Precursor Solvate Phases

Solution-processed hybrid perovskite semiconductors attract a great deal of attention, but little is known about their formation process. The one-step spin-coating process of perovskites is investigated in situ, revealing that thin-film formation is mediated by solid-state precursor solvates and their nature. The stability of these intermediate phases directly impacts the quality and reproducibility of thermally converted perovskite films and their photovoltaic performance.

Solid‐State Processing of Organic Semiconductors

By Mohammed A. Baklar , elix F Koch , Avinesh Kumar , Ester Buchaca Domingo , Mariano Campoy-Quiles , Kirill eldman , F Liyang u , Y Paul Wobkenberg , James Ball , Rory M. Wilson , Iain McCulloch , Theo Kreouzis , Martin Heeney , Thomas Anthopoulos , Paul Smith ,

Entanglements in marginal solutions: a means of tuning pre-aggregation of conjugated polymers with positive implications for charge transport

The solution-processing of conjugated polymers, just like commodity polymers, is subject to solvent and molecular weight-dependent solubility, interactions and chain entanglements within the polymer, all of which can influence the crystallization and microstructure development in semi-crystalline polymers and consequently affect charge transport and optoelectronic properties. Disentanglement of polymer chains in marginal solvents was reported to work via ultrasonication, facilitating the formation of photophysically ordered polymer aggregates. In this contribution, we explore how a wide range of technologically relevant solvents and formulations commonly used in organic electronics influence chain entanglement and the aggregation behaviour of P3HT using a combination of rheological and spectrophotometric measurements. The specific viscosity of the solution offers an excellent indication of the degree of entanglements in the solution, which is found to be related to the solubility of P3HT in a given solvent. Moreover, deliberately disentangling the solution in the presence of solvophobic driving forces, leads consistently to formation of photophysically visible aggregates which is indicative of local and perhaps long range order in the solute. We show for a broad range of solvents and molecular weights that disentanglement ultimately leads to significant ordering of the polymer in the solid state and a commensurate increase in charge transport properties. In doing so we demonstrate a remarkable ability to tune the microstructure which has important implications for transport properties. We discuss its potential implications in the context of organic electronics and photovoltaics.

Wire-bar coating of semiconducting polythiophene/insulating polyethylene blend thin films for organic transistors

Organic blend thin films consisting of semiconducting poly(3-hexylthiophene) (P3HT) and insulating high-density polyethylene (HDPE) have been fabricated by novel application of a large area wire-bar coating technique in air. The microstructure of P3HT:HDPE blend films reveals a strong structural dependence on initial composition. Preferential segregation of P3HT toward the film surface is observed for all blend compositions, while P3HT (or P3HT-rich) columnar structures enclosed by HDPE (or HDPE-rich) lamellar matrix is distinctive for 50:50 (by weight) blends. The transistors fabricated with P3HT:HDPE blend films show a clear field effect behavior, exhibiting charge carrier mobilities up to 5 × 10−2 cm2/Vs, comparable to the values reported in spin-coated similar blends and of neat P3HT devices. The wire-bar coated blend films and devices are highly repeatable and spatially uniform over large areas (few cm by few cm), demonstrating the suitability of this technique for manufacturing of large area organic...

Highly efficient polymer solar cells with printed photoactive layer: rational process transfer from spin-coating

Scalable and continuous roll-to-roll manufacturing is at the heart of the promise of low-cost and high throughput manufacturing of solution-processed photovoltaics. Yet, to date the vast majority of champion organic solar cells reported in the literature rely on spin-coating of the photoactive bulk heterojunction (BHJ) layer, with the performance of printed solar cells lagging behind in most instances. Here, we investigate the performance gap between polymer solar cells prepared by spin-coating and blade-coating the BHJ layer for the important class of modern polymers exhibiting no long range crystalline order. We find that thickness parity does not always yield performance parity even when using identical formulations. Significant differences in the drying kinetics between the processes are found to be responsible for BHJ nanomorphology differences. We propose an approach which benchmarks the film drying kinetics and associated BHJ nanomorphology development against those of the champion laboratory devices prepared by spin-coating the BHJ layer by adjusting the process temperature. If the optimization requires the solution concentration to be changed, then it is crucial to maintain the additive-to-solute volume ratio. Emulating the drying kinetics of spin-coating is also shown to help achieve morphological and performance parities. We put this approach to the test and demonstrate printed PTB7:PC71BM polymer solar cells with efficiency of 9% and 6.5% PCEs on glass and flexible PET substrates, respectively. We further demonstrate performance parity for two other popular donor polymer systems exhibiting rigid backbones and absence of a long range crystalline order, achieving a PCE of 9.7%, the highest efficiency reported to date for a blade coated organic solar cell. The rational process transfer illustrated in this study should help the broader and successful adoption of scalable printing methods for these material systems.

Polar Side Chains Enhance Processability, Electrical Conductivity, and Thermal Stability of a Molecularly p-Doped Polythiophene.

Molecular doping of organic semiconductors is critical for optimizing a range of optoelectronic devices such as field-effect transistors, solar cells, and thermoelectric generators. However, many dopant:polymer pairs suffer from poor solubility in common organic solvents, which leads to a suboptimal solid-state nanostructure and hence low electrical conductivity. A further drawback is the poor thermal stability through sublimation of the dopant. The use of oligo ethylene glycol side chains is demonstrated to significantly improve the processability of the conjugated polymer p(g4 2T-T)-a polythiophene-in polar aprotic solvents, which facilitates coprocessing of dopant:polymer pairs from the same solution at room temperature. The use of common molecular dopants such as 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4TCNQ) and 2,3-dichloro-5,6-dicyano-1,4-benzoquinone (DDQ) is explored. Doping of p(g4 2T-T) with F4TCNQ results in an electrical conductivity of up to 100 S cm-1 . Moreover, the increased compatibility of the polar dopant F4TCNQ with the oligo ethylene glycol functionalized polythiophene results in a high degree of thermal stability at up to 150 °C.

Single-step solution processing of small-molecule organic semiconductor field-effect transistors at high yield

Here, we report a simple, alternative route towards high-mobility structures of the small-molecular semiconductor 5,11-bis(triethyl silylethynyl) anthradithiophene that requires one single processing step without the need for any post-deposition processing. The method relies on careful control of the casting temperature of the semiconductor and allows rapid production of transistors with uniform and reproducible device performance over large areas.

Solution-processed small molecule transistors with low operating voltages and high grain-boundary anisotropy

We present a new soluble pentacene derivative with ethyl substitutions in the 1,13,14,22 backbone positions to modulate the solubility and film forming properties of this material compared to triisopropylsilylethynyl (TIPS) pentacene. This permits reproducible production of molecularly highly ordered structures that feature average transistor mobilities in excess of 1 cm2 V−1 s−1 depending on crystal orientation by careful selection of casting conditions.