Effect of organic electroactive crystallites in a dielectric matrix on the electrical properties of a polymer dielectric

Lee, Taein; Luo, Yi; Wang, Chuhong; Park, A.; Zapata-Mercado, Elmer; Hristova, Kalina; Mueller, Timothy I.; Wilson, William L.; Reich, Daniel H.; Katz, Howard E.

doi:10.1103/physrevmaterials.7.065003

Cited by 3 publications

(3 citation statements)

References 44 publications

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“…However, for PS- b -PAAS, the behavior was different, where widely scattered larger crystallites were well formed at 5%, and as the concentration was increased, more such crystallites were formed with similar size and appearance. From our experience, what happened in the PS/2AA film was also observed when other crystallizable small molecules, e.g., α-quaterthiophene, were blended and spin-coated with polymers . For the pure PS- b -PAAS film, similar behavior was not found by OM; in particular, submicrometer crystallites were not observed.…”

Section: Resultsmentioning

confidence: 99%

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2-Aminoanthracene Crystallization in Its Compatible Polystyrene Block: RAFT Synthesis and Enhanced Charge Retention in Pentacene Transistor Gate Dielectrics

Chi,

Song,

Lee

et al. 2023

Macromolecules

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We synthesized polystyrene-block-polyanthrylaminomethylstyrene (PS-b-PAAS) via the RAFT reaction and side chain modification, where the PAAS block is 50%. By blending 2-aminoanthracene (2AA) with PS-b-PAAS, the coaggregation behavior of the PAAS block and 2AA within the thin film was observed by optical microscopy (OM) and X-ray diffraction. At 5 and 10 wt % 2AA within the thin film, OM results showed a clear morphological difference between the PS matrix and PS-b-PAAS matrix. Differences in the 2AA excited-state lifetimes in these matrices were also established by using transient absorption spectroscopy (TAS). Blends were used as gate dielectrics in the pentacene transistors. We compared characteristic voltage (V c, an indicator of threshold voltage) before and after charging of PS-b-PAAS blended with unsubstituted PS and both polymers individually blended with 2AA. For blended PS-b-PAAS and PS, as the concentration of PS-b-PAAS increases, the decreased Vc especially with negative charging of the pentacene indicated a larger concentration of charge carriers induced by the dielectric film. The charging experiments also revealed that the unique structure formed by the 2AA/PS-b-PAAS blend significantly affected the charge storage capability of organic field-effect transistors (OFETs). This work demonstrates the novel coaggregation structure in the dielectrics and furthermore its impact on charge storage capability in pentacene OFETs.

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Section: Resultsmentioning

confidence: 99%

“…From our experience, what happened in the PS/2AA film was also observed when other crystallizable small molecules, e.g., αquaterthiophene, were blended and spin-coated with polymers. 23 For the pure PS-b-PAAS film, similar behavior was not found by OM; in particular, submicrometer crystallites were not observed.…”

Section: Polymer Design and Synthesismentioning

confidence: 99%

2-Aminoanthracene Crystallization in Its Compatible Polystyrene Block: RAFT Synthesis and Enhanced Charge Retention in Pentacene Transistor Gate Dielectrics

Chi,

Song,

Lee

et al. 2023

Macromolecules

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“…All these factors affect the molecular packing of deposited material. The alignment in molecular packing results in a reduction in pi-pi stacking distance and hence an increase in charge transport [24][25][26]. So, for long-range alignment of the molecular backbone and side chains, controlled deposition techniques are required and nano-patterning of the substrate prior to polymer deposition is a potential directional deposition technique among them [27,28].…”

Section: Introductionmentioning

confidence: 99%

Long-range polymer ordering by directional coating to remarkably enhance the charge carrier mobility in PCDTPT-based organic field-effect transistors

Iqbal,

Saghir,

Afzal

et al. 2024

R. Soc. Open Sci.

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With the wide potential of organic field-effect transistors in all the modern electronic circuitries, researchers are grappling with the challenge of poor charge transport and hence lower mobility in organic polymers. Low-charge carrier mobility is mainly due to disorder in the molecular packing of organic semiconductors along with other factors, such as impurities, defects and interactions between molecules. The current research work has been conducted to align the molecular chains of poly[4-(4,4-dihexadecyl-4H-cyclopenta[1,2-‌‌‌b:5,4-‌b′]‌dithiophen-2-yl)-alt-[1,2,5]thiadiazolo-[3,4-c]pyridine] (PCDTPT) using directional coating techniques such as dip coating and brush coating on nano-grooved substrates. Long-range order of polymer chains was clearly observed along the direction of brush coating and nanogrooves in optical and atomic force microscope (AFM) images while transmission spectra confirmed decreased pi–pi stacking for the polymer films deposited by this technique. By comparing the mobility performance of brush-coated devices with other techniques, we found a remarkable mobility enhancement of 90 times that of conventional spin-coated device and 24 times enhancement compared with the dip-coated device for the case when the alignment of polymer chains was parallel to the channel. All the fabrication and characterizations were performed in the ambient environment. This study demonstrates a potential approach to align the polymers on long and short ranges hence providing a route for high-performing devices in ambient conditions.

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Increased Static Charge‐Induced Threshold Voltage Shifts and Memristor Activity in Pentacene OFETs Comprising Polystyrene‐Based Gate Dielectrics Containing Electroactive Small Molecule Crystallites

Bond,

Reich,

Katz

2024

Adv Funct Materials

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Top‐contact bottom‐gate pentacene OFETs are fabricated with single layer dielectrics comprised of either polystyrene (PS), poly(4‐methylstyrene) (P4MS), or poly(4‐tert‐butylstyrene) (P4TBS). The polystyrenes are blended with varying concentrations of two different small molecules, dibenzotetrathiafulvalene (DBTTF) and 2,8‐difluoro‐5,11‐bis(triethylsilylethynyl)anthradithiophene (diF‐TES‐ADT), to form small, separated crystallites contained throughout the polymer dielectric layer. The OFET characteristics of these devices are investigated and their threshold voltage shifts are measured after −70 V static charging for 5 min. Two‐terminal measurements are conducted using multiple different gate biases in the range of −50 to +50 V to investigate memristor behavior in the devices. OFETs containing DBTTF exhibited ΔVth increases as large as 330% relative to control OFETs containing no DBTTF, while OFETs containing at least 7.5 wt.% DBTTF exhibited memristor activity, with currents ranging from 20 nA to 44 µA depending on the applied bias. This work demonstrates that including small, separated crystallites in polymer dielectrics enhances their charge storage ability and can be promising for creating nonbinary memory devices for data processing. Additionally, the observed memristor activity indicates the OFETs in this work can be used in development of neuromorphic systems that aim to mimic the synaptic behavior of the human nervous system.

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Effect of organic electroactive crystallites in a dielectric matrix on the electrical properties of a polymer dielectric

Cited by 3 publications

References 44 publications

2-Aminoanthracene Crystallization in Its Compatible Polystyrene Block: RAFT Synthesis and Enhanced Charge Retention in Pentacene Transistor Gate Dielectrics

2-Aminoanthracene Crystallization in Its Compatible Polystyrene Block: RAFT Synthesis and Enhanced Charge Retention in Pentacene Transistor Gate Dielectrics

Long-range polymer ordering by directional coating to remarkably enhance the charge carrier mobility in PCDTPT-based organic field-effect transistors

Increased Static Charge‐Induced Threshold Voltage Shifts and Memristor Activity in Pentacene OFETs Comprising Polystyrene‐Based Gate Dielectrics Containing Electroactive Small Molecule Crystallites

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