| 1. |
- Gerasimov, Jennifer Yevgenia, 1985-, et al.
(author)
-
Rational Materials Design for In Operando Electropolymerization of Evolvable Organic Electrochemical Transistors
- 2022
-
In: Advanced Functional Materials. - : John Wiley and Sons Inc. - 1616-301X .- 1616-3028. ; 32
-
Journal article (peer-reviewed)abstract
- Organic electrochemical transistors formed by in operando electropolymerization of the semiconducting channel are increasingly becoming recognized as a simple and effective implementation of synapses in neuromorphic hardware. However, very few studies have reported the requirements that must be met to ensure that the polymer spreads along the substrate to form a functional conducting channel. The nature of the interface between the substrate and various monomer precursors of conducting polymers through molecular dynamics simulations is investigated, showing that monomer adsorption to the substrate produces an increase in the effective monomer concentration at the surface. By evaluating combinatorial couples of monomers baring various sidechains with differently functionalized substrates, it is shown that the interactions between the substrate and the monomer precursor control the lateral growth of a polymer film along an inert substrate. This effect has implications for fabricating synaptic systems on inexpensive, flexible substrates. © 2022 The Authors.
|
|
| 2. |
- Andersson Ersman, Peter, et al.
(author)
-
All-printed large-scale integrated circuits based on organic electrochemical transistors
- 2019
-
In: Nature Communications. - : Nature Publishing Group. - 2041-1723. ; 10:1
-
Journal article (peer-reviewed)abstract
- The communication outposts of the emerging Internet of Things are embodied by ordinary items, which desirably include all-printed flexible sensors, actuators, displays and akin organic electronic interface devices in combination with silicon-based digital signal processing and communication technologies. However, hybrid integration of smart electronic labels is partly hampered due to a lack of technology that (de)multiplex signals between silicon chips and printed electronic devices. Here, we report all-printed 4-to-7 decoders and seven-bit shift registers, including over 100 organic electrochemical transistors each, thus minimizing the number of terminals required to drive monolithically integrated all-printed electrochromic displays. These relatively advanced circuits are enabled by a reduction of the transistor footprint, an effort which includes several further developments of materials and screen printing processes. Our findings demonstrate that digital circuits based on organic electrochemical transistors (OECTs) provide a unique bridge between all-printed organic electronics (OEs) and low-cost silicon chip technology for Internet of Things applications. © 2019, The Author(s).
|
|
| 3. |
- Chen, Shangzhi, et al.
(author)
-
Conductive polymer nanoantennas for dynamic organic plasmonics
- 2020
-
In: Nature Nanotechnology. - London : Nature Publishing Group. - 1748-3387 .- 1748-3395. ; 15
-
Journal article (peer-reviewed)abstract
- Being able to dynamically shape light at the nanoscale is oneof the ultimate goals in nano-optics1. Resonant light–matterinteraction can be achieved using conventional plasmonicsbased on metal nanostructures, but their tunability is highlylimited due to a fixed permittivity2. Materials with switchablestates and methods for dynamic control of light–matterinteraction at the nanoscale are therefore desired. Here weshow that nanodisks of a conductive polymer can supportlocalized surface plasmon resonances in the near-infraredand function as dynamic nano-optical antennas, with their resonancebehaviour tunable by chemical redox reactions. Theseplasmons originate from the mobile polaronic charge carriersof a poly(3,4-ethylenedioxythiophene:sulfate) (PEDOT:Sulf)polymer network. We demonstrate complete and reversibleswitching of the optical response of the nanoantennasby chemical tuning of their redox state, which modulatesthe material permittivity between plasmonic and dielectricregimes via non-volatile changes in the mobile chargecarrier density. Further research may study different conductivepolymers and nanostructures and explore their usein various applications, such as dynamic meta-optics andreflective displays.
|
|
| 4. |
- Darabi, Sozan, 1994, et al.
(author)
-
Polymer-Based n-Type Yarn for Organic Thermoelectric Textiles
- 2023
-
In: Advanced Electronic Materials. - : Wiley. - 2199-160X .- 2199-160X. ; 9:4
-
Journal article (peer-reviewed)abstract
- A conjugated-polymer-based n-type yarn for thermoelectric textiles is presented. Thermoelectric textile devices are intriguing power sources for wearable electronic devices. The use of yarns comprising conjugated polymers is desirable because of their potentially superior mechanical properties compared to other thermoelectric materials. While several examples of p-type conducting yarns exist, there is a lack of polymer-based n-type yarns. Here, a regenerated cellulose yarn is spray-coated with an n-type conducting-polymer-based ink composed of poly(benzimidazobenzophenanthroline) (BBL) and poly(ethyleneimine) (PEI). The n-type yarns display a bulk electrical conductivity of 8 × 10−3 S cm−1 and Seebeck coefficient of −79 µV K−1. A promising level of air-stability for at least 13 days can be achieved by applying an additional thermoplastic elastomer coating. A prototype in-plane thermoelectric textile, produced with the developed n-type yarns and p-type yarns, composed of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS)-coated regenerated cellulose, displays a stable device performance in air for at least 4 days with an open-circuit voltage per temperature difference of 1 mV °C−1. Evidently, polymer-based n-type yarns are a viable component for the construction of thermoelectric textile devices.
|
|
| 5. |
- Fahlman, Mats, 1967-, et al.
(author)
-
Interfaces in organic electronics
- 2019
-
In: Nature Reviews Materials. - : Nature Publishing Group. - 2058-8437. ; 4:10, s. 627-650
-
Research review (peer-reviewed)abstract
- Undoped, conjugated, organic molecules and polymers possess properties of semiconductors, including the electronic structure and charge transport, which can be readily tuned by chemical design. Moreover, organic semiconductors (OSs) can be n-doped or p-doped to become organic conductors and can exhibit mixed electronic and ionic conductivity. Compared with inorganic semiconductors and metals, organic (semi)conductors possess a unique feature: no insulating oxide forms on their surface when exposed to air. Thus, OSs form clean interfaces with many materials, including metals and other OSs. OS–metal and OS–OS interfaces have been intensely investigated over the past 30 years, from which a consistent theoretical description has emerged. Since the 2000s, increased attention has been paid to interfaces in organic electronics that involve dielectrics, electrolytes, ferroelectrics and even biological organisms. In this Review, we consider the central role of these interfaces in the function of organic electronic devices and discuss how the physico-chemical properties of the interfaces govern the interfacial transport of light, excitons, electrons and ions, as well as the transduction of electrons into the molecular language of cells.
|
|
| 6. |
- Guo, Han, et al.
(author)
-
Transition metal-catalysed molecular n-doping of organic semiconductors
- 2021
-
In: Nature. - London, United Kingdom : Nature Publishing Group. - 0028-0836 .- 1476-4687. ; 599:7883, s. 67-73
-
Journal article (peer-reviewed)abstract
- Electron doping of organic semiconductors is typically inefficient, but here a precursor molecular dopant is used to deliver higher n-doping efficiency in a much shorter doping time. Chemical doping is a key process for investigating charge transport in organic semiconductors and improving certain (opto)electronic devices(1-9). N(electron)-doping is fundamentally more challenging than p(hole)-doping and typically achieves a very low doping efficiency (eta) of less than 10%(1,10). An efficient molecular n-dopant should simultaneously exhibit a high reducing power and air stability for broad applicability(1,5,6,9,11), which is very challenging. Here we show a general concept of catalysed n-doping of organic semiconductors using air-stable precursor-type molecular dopants. Incorporation of a transition metal (for example, Pt, Au, Pd) as vapour-deposited nanoparticles or solution-processable organometallic complexes (for example, Pd-2(dba)(3)) catalyses the reaction, as assessed by experimental and theoretical evidence, enabling greatly increased eta in a much shorter doping time and high electrical conductivities (above 100 S cm(-1); ref. (12)). This methodology has technological implications for realizing improved semiconductor devices and offers a broad exploration space of ternary systems comprising catalysts, molecular dopants and semiconductors, thus opening new opportunities in n-doping research and applications(12, 13).
|
|
| 7. |
- Han, Shaobo, et al.
(author)
-
A Multiparameter Pressure–Temperature–Humidity Sensor Based on Mixed Ionic–Electronic Cellulose Aerogels
- 2019
-
In: Advanced Science. - : Wiley. - 2198-3844.
-
Journal article (peer-reviewed)abstract
- Pressure (P), temperature (T), and humidity (H) are physical key parameters of great relevance for various applications such as in distributed diagnostics, robotics, electronic skins, functional clothing, and many other Internet-of-Things (IoT) solutions. Previous studies on monitoring and recording these three parameters have focused on the integration of three individual single-parameter sensors into an electronic circuit, also comprising dedicated sense amplifiers, signal processing, and communication interfaces. To limit complexity in, e.g., multifunctional IoT systems, and thus reducing the manufacturing costs of such sensing/communication outposts, it is desirable to achieve one single-sensor device that simultaneously or consecutively measures P–T–H without cross-talks in the sensing functionality. Herein, a novel organic mixed ion–electron conducting aerogel is reported, which can sense P–T–H with minimal cross-talk between the measured parameters. The exclusive read-out of the three individual parameters is performed electronically in one single device configuration and is enabled by the use of a novel strategy that combines electronic and ionic Seebeck effect along with mixed ion–electron conduction in an elastic aerogel. The findings promise for multipurpose IoT technology with reduced complexity and production costs, features that are highly anticipated in distributed diagnostics, monitoring, safety, and security applications. © 2019 The Authors.
|
|
| 8. |
- Han, Shaobo, 1988-
(author)
-
Thermoelectric polymer-cellulose composite aerogels
- 2019
-
Doctoral thesis (other academic/artistic)abstract
- Thermoelectric materials are scrutinized as energy materials and sensing materials. Indeed, they convert thermal energy into electrical energy. In addition, those materials are actively sensitive to a temperature modification through the generation of an electric signal. Organic thermoelectric (OTE) materials are complementary to inorganic thermoelectric materials, as they possess unique properties such as solution processing, ionic conductivity, flexibility, and softness. While thin-film OTE materials have been widely studied because they are easily manufactured by various coating techniques, little is done in the creation of three-dimensional morphologies of OTE materials; which is important to develop large temperature gradients.Cellulose is the most abundant biopolymer on the planet. Recently, the applications of cellulose are not only limited in making papers but also in electronics as the cellulose provide 3-D microstructures and mechanical strength. One promising approach to make 3-D OTE bulks is using cellulose as scaffold because of their properties of relatively high mechanical strength, water processability and environmentally friendly performance.The aims of the thesis have been to enlarge the applications of an OTE material poly(3,4-ethylenedioxythiophene) (PEDOT), with an approach of making 3-D aerogels composite with nanofibrillated cellulose (NFC), in two main areas: (1) multi-parameter sensors and (2) solar vapor generators. In the first application, we demonstrate that the new thermoelectric aerogel responds independently to pressure P, temperature T and humidity RH. Hence, when it is submitted to the three stresses (T, P, RH), the electrical characterization of the material enables to measure the three parameters without cross-talking effects. Thermoelectric aerogels are foreseen as active materials in electronic skins and robotics. In the second application, the conducting polymer aerogels are employed as solar absorbers to convert solar energy into heat and significantly increased the water evaporation rate. The IR absorption is efficient because of the free-electron in the conducting polymer PEDOT nano-aggregates. Because of the low cost of those materials and the water stability of the crosslinked aerogels, they could be of importance for water desalination.
|
|
| 9. |
- Jiang, Qinglin, et al.
(author)
-
High Thermoelectric Performance in n-Type Perylene Bisimide Induced by the Soret Effect
- 2020
-
In: Advanced Materials. - : WILEY-V C H VERLAG GMBH. - 0935-9648 .- 1521-4095. ; 32:45
-
Journal article (peer-reviewed)abstract
- Low-cost, non-toxic, abundant organic thermoelectric materials are currently under investigation for use as potential alternatives for the production of electricity from waste heat. While organic conductors reach electrical conductivities as high as their inorganic counterparts, they suffer from an overall low thermoelectric figure of merit (ZT) due to their small Seebeck coefficient. Moreover, the lack of efficient n-type organic materials still represents a major challenge when trying to fabricate efficient organic thermoelectric modules. Here, a novel strategy is proposed both to increase the Seebeck coefficient and achieve the highest thermoelectric efficiency for n-type organic thermoelectrics to date. An organic mixed ion-electron n-type conductor based on highly crystalline and reduced perylene bisimide is developed. Quasi-frozen ionic carriers yield a large ionic Seebeck coefficient of -3021 mu V K-1, while the electronic carriers dominate the electrical conductivity which is as high as 0.18 S cm(-1)at 60% relative humidity. The overall power factor is remarkably high (165 mu W m(-1)K(-2)), with aZT= 0.23 at room temperature. The resulting single leg thermoelectric generators display a high quasi-constant power output. This work paves the way for the design and development of efficient organic thermoelectrics by the rational control of the mobility of the electronic and ionic carriers.
|
|
| 10. |
- Li, Zaifang, et al.
(author)
-
A Free-Standing High-Output Power Density Thermoelectric Device Based on Structure-Ordered PEDOT:PSS
- 2018
-
In: Advanced Electronic Materials. - : Wiley-VCH Verlagsgesellschaft. - 2199-160X. ; 4:2
-
Journal article (peer-reviewed)abstract
- A free-standing high-output power density polymeric thermoelectric (TE) device is realized based on a highly conductive (approximate to 2500 S cm(-1)) structure-ordered poly(3,4-ethylenedioxythiophene):polystyrene sulfonate film (denoted as FS-PEDOT:PSS) with a Seebeck coefficient of 20.6 mu V K-1, an in-plane thermal conductivity of 0.64 W m(-1) K-1, and a peak power factor of 107 mu W K-2 m(-1) at room temperature. Under a small temperature gradient of 29 K, the TE device demonstrates a maximum output power density of 99 +/- 18.7 mu W cm(-2), which is the highest value achieved in pristine PEDOT:PSS based TE devices. In addition, a fivefold output power is demonstrated by series connecting five devices into a flexible thermoelectric module. The simplicity of assembling the films into flexible thermoelectric modules, the low out-of-plane thermal conductivity of 0.27 W m(-1) K-1, and free-standing feature indicates the potential to integrate the FS-PEDOT:PSS TE modules with textiles to power wearable electronics by harvesting human bodys heat. In addition to the high power factor, the high thermal stability of the FS-PEDOT:PSS films up to 250 degrees C is confirmed by in situ temperature-dependent X-ray diffraction and grazing incident wide angle X-ray scattering, which makes the FS-PEDOT:PSS films promising candidates for thermoelectric applications.
|
|
| 11. |
- Makhinia, Anatolii
(author)
-
Advances in Additive Manufacturing of Organic Electrochemical Transistors
- 2024
-
Doctoral thesis (other academic/artistic)abstract
- Technological advances and applications of printed electronic devices rely on novel organic semiconductor (OSC) materials and cutting-edge advanced manufacturing technologies. A growing number of solution- processable organic electronic materials has paved the way towards cost- efficient fabrication techniques, fostering the growth and emergence of printed electronics research in recent decades. Organic semiconductor materials are unique because of mixed ionic and electronic transport of charges that may translate biological signals into electrical ones or vice versa. The organic electrochemical transistor (OECT) is a type of transistor where the active material (channel) is made of an organic mixed ionic-electronic conductor (OMIEC). Since OECTs may serve as organic bioelectronic devices that encompass high ionic and electronic conductivity, they also represent a groundbreaking technology by forming communication channels between living systems and external electronic circuits used for recording. Highly conductive and stable OMIECs, sustainable solvents for ink formulations, bio-based substrates, new device architectures and redefined manufacturing strategies are the keys that unlock highly sensitive OECT-based (bio)sensor devices and OECT-based electronic circuits with high gain and low power consumption. This dissertation explores and unveils the effects of different additive manufacturing strategies, channel materials, ink formulations and device architectures on the performance and applications of all-printed OECT devices. The key findings of this thesis are summarized in four first-authored scientific journal articles. In the first article, we redefined the manufacturing approach to create high performance all-printed OECTs exhibiting very short switching times; this approach was further verified by printing OECT-based inverters operating at a frequency beyond 100 Hz and five-stage ring oscillators. In the second article, we developed an all-printed sensor platform by combining highly sensitive OECT and piezoelectric sensor devices on a tattoo paper substrate for seamless integration with the skin, enabling the detection of radial pulse waves. In the third article, a screen printed OECT was integrated into capillary 3D-printed microfluidics with the goal of ion sensing, thereby forming an additively manufactured sensor platform. The fourth article demonstrates, for the first time, vertically stacked accumulation mode pgBTTT-based OECTs manufactured by combining screen and inkjet printing technologies. By selecting a non-toxic and biodegradable solvent (Cyrene) instead of chloroform in the preparation of the pgBTTT-based inkjet ink formulation, we move towards more sustainable OECTs. The resulting all-printed pgBTTT-based OECTs exhibited high figures of merit, short switching times and good operational stability in an ambient environment. Finally, this dissertation offers insights and perspectives on the rational use of printing technologies, channel materials (p-type), sustainable ink formulations, and device architectures to enable further progress of all-printed OECT-based (bio)sensors, amplifiers and complementary logic circuits for various (bio)electronic applications.
|
|
| 12. |
- Shiran Chaharsoughi, Mina, 1986-, et al.
(author)
-
Hybrid Plasmonic and Pyroelectric Harvesting of Light Fluctuations
- 2018
-
In: Advanced Optical Materials. - : Wiley-Blackwell. - 2162-7568 .- 2195-1071.
-
Journal article (peer-reviewed)abstract
- State-of-the-art solar energy harvesting systems based on photovoltaic technology require constant illumination for optimal operation. However, weather conditions and solar illumination tend to fluctuate. Here, a device is presented that extracts electrical energy from such light fluctuations. The concept combines light-induced heating of gold nanodisks (acting as plasmonic optical nanoantennas), and an organic pyroelectric copolymer film (poly(vinylidenefluoride-co-trifluoroethylene)), that converts temperature changes into electrical signals. This hybrid device can repeatedly generate current pulses, not only upon the onset of illumination, but also when illumination is blocked. Detailed characterization highlights the key role of the polarization state of the copolymer, while the copolymer thickness has minor influence on performance. The results are fully consistent with plasmon-assisted pyroelectric effects, as corroborated by combined optical and thermal simulations that match the experimental results. Owing to the tunability of plasmonic resonances, the presented concept is compatible with harvesting near infrared light while concurrently maintaining visible transparency.
|
|
| 13. |
- Shiran Chaharsoughi, Mina, 1986-
(author)
-
Hybrid Plasmonics for Energy Harvesting and Sensing of Radiation and Heat
- 2020
-
Doctoral thesis (other academic/artistic)abstract
- The special optical properties of subwavelength metallic structures have opened up for numerous applications in different fields. The interaction of light with metal nanostructures leads to the excitation of collective oscillations of conduction-band electrons, known as plasmons. These plasmon excitations are responsible for the high absorption and high scattering of light in metallic nanostructures. High absorption of light and the subsequent temperature increase in the nanostructures make them suitable as point-like heat sources that can be controlled remotely by light.The research presented in this thesis focuses on the development and studies of hybrid devices that combine light-induced heating in plasmonic nanostructures with other materials and systems. Particular focus is put on hybrid organic-inorganic systems for applications in energy harvesting as well as in heat and radiation sensing. Harvesting energy from light fluctuations was achieved in a hybrid device consisting of plasmonic gold nanodisk arrays and a pyroelectric copolymer. In this concept, fast and efficient light-induced heating in the gold nanodisks modulated the temperature of the pyroelectric layer, which could be used to extract electrical energy from fluctuations in simulated sunlight.Integrating plasmonic nanostructures with complementary materials can also provide novel hybrid sensors, for monitoring of temperature, heat flux and radiation. In this thesis work, a hybrid sensor was designed based on the combination of a plasmonic gold nanohole layer with a pyroelectric copolymer and an ionic thermoelectric gel. The gold nanohole arrays acted both as broadband light absorbers in the visible to near-infrared spectral range of the solar spectrum and also as one of the electrodes of the sensor. In contrast to the constituent components when used separately, the hybrid sensor could provide both fast and stable signals upon heat or radiation stimuli, as well as enhanced equilibrium signals.Furthermore, a concept for heat and radiation mapping was developed that was highly sensitive and stable despite its simple structure. The concept consisted of a gel-like electrolyte connecting two separated metal nanohole electrodes on a substrate. Resembling traditional thermocouples, this concept could autonomously detect temperature changes but with several orders of magnitudes higher sensitivity. Owing to its promising sensing properties as well as its compatibility with inexpensive mass production methods on flexible substrates, such concept may be particularly interesting for electronic skin applications for health monitoring and for humanoid robotics. Finally, we improved the possibilities for the temperature mapping of the concept by modifying the structure from lateral to vertical form. Similar to the lateral device, the vertical temperature sensor showed high temperature sensitivity and stability in producing signals upon temperature changes.
|
|
| 14. |
- Wang, Gang, et al.
(author)
-
Photovoltaic Blend Microstructure for High Efficiency Post-Fullerene Solar Cells. To Tilt or Not To Tilt?
- 2019
-
In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 141:34, s. 13410-13420
-
Journal article (peer-reviewed)abstract
- Achieving efficient polymer solar cells (PSCs) requires a structurally optimal donor-acceptor heterojunction morphology. Here we report the combined experimental and theoretical characterization of a benzodithiophene-benzo-thiadiazole donor polymer series (PBTZF4-R; R = alkyl substituent) blended with the non-fullerene acceptor ITIC-Th and analyze the effects of substituent dimensions on blend morphology, charge transport, carrier dynamics, and PSC metrics. Varying substituent dimensions has a pronounced effect on the blend morphology with a direct link between domain purity, to some extent domain dimensions, and charge generation and collection. The polymer with the smallest alkyl substituent yields the highest PSC power conversion efficiency (PCE, 11%), reflecting relatively small, high-purity domains and possibly benefiting from "matched" donor polymer-small molecule acceptor orientations. The distinctive morphologies arising from the substituents are investigated using molecular dynamics (MD) simulations which reveal that substituent dimensions dictate a well-defined set of polymer conformations, in turn driving chain aggregation and, ultimately, the various film morphologies and mixing with acceptor small molecules. A straightforward energetic parameter explains the experimental polymer domain morphological trends, hence PCE, and suggests strategies for substituent selection to optimize PSC materials morphologies.
|
|
| 15. |
- Xu, Kai, et al.
(author)
-
On the Origin of Seebeck Coefficient Inversion in Highly Doped Conducting Polymers
- 2022
-
In: Advanced Functional Materials. - : Wiley-V C H Verlag GMBH. - 1616-301X .- 1616-3028. ; 32:20
-
Journal article (peer-reviewed)abstract
- A common way of determining the majority charge carriers of pristine and doped semiconducting polymers is to measure the sign of the Seebeck coefficient. However, a polarity change of the Seebeck coefficient has recently been observed to occur in highly doped polymers. Here, it is shown that the Seebeck coefficient inversion is the result of the density of states filling and opening of a hard Coulomb gap around the Fermi energy at high doping levels. Electrochemical n-doping is used to induce high carrier density (>1 charge/monomer) in the model system poly(benzimidazobenzophenanthroline) (BBL). By combining conductivity and Seebeck coefficient measurements with in situ electron paramagnetic resonance, UV-vis-NIR, Raman spectroelectrochemistry, density functional theory calculations, and kinetic Monte Carlo simulations, the formation of multiply charged species and the opening of a hard Coulomb gap in the density of states, which is responsible for the Seebeck coefficient inversion and drop in electrical conductivity, are uncovered. The findings provide a simple picture that clarifies the roles of energetic disorder and Coulomb interactions in highly doped polymers and have implications for the molecular design of next-generation conjugated polymers.
|
|
| 16. |
- Zhang, Qilun, 1992-, et al.
(author)
-
Natural Product Betulin-Based Insulating Polymer Filler in Organic Solar Cells
- 2022
-
In: Solar RRL. - : Wiley. - 2367-198X. ; 6:9
-
Journal article (peer-reviewed)abstract
- Introduction of filler materials into organic solar cells (OSCs) are a promising strategy to improve device performance and thermal/mechanical stability. However, the complex interactions between the state-of-the-art OSC materials and filler require careful selection of filler materials and OSC fabrication to achieve lower cost and improved performance. In this work, the introduction of a natural product betulin-based insulating polymer as filler in various OSCs is investigated. Donor–acceptor–insulator ternary OSCs are developed with improved open-circuit voltage (Voc) due to decreased trap-assisted recombination. Furthermore, filler-induced vertical phase separation due to mismatched surface energy can strongly affect charge collection at the bottom interface and limit the filler ratio. A quasi-bilayer strategy is used in all-polymer systems to circumvent this problem. Herein, the variety of filler materials in OSCs to biomass is broadened, and the filler strategy is made a feasible and promising strategy toward highly efficient, eco, and low-cost OSCs.
|
|
| 17. |
- Zhang, Silan, 1992-
(author)
-
Organic Electrochemical Transistors : Materials and Challenges
- 2023
-
Doctoral thesis (other academic/artistic)abstract
- The use of organic mixed ionic-electronic conductors (OMIECs) has demonstrated the potential to transform the field of bioelectronics, spanning from medical diagnostics to neuromorphic computing hardware. To keep up with the fast-paced demands, it is crucial to develop customizable device fabrication, design new materials, improve operation stability, and explore the ion-electron interactions within OMIECs. This thesis explores the application of OMIECs in organic electrochemical transistors (OECTs), a crucial component of a range of organic bioelectronic devices. To meet applications requiring rapid design iterations and leveraging digitally enabled direct-write techniques, we developed a novel approach for fabricating fully 3D-printed OECTs using a direct-write additive process. This method involves utilizing 3D printable inks with conductive, semiconductive, insulating, and electrolyte properties. The resulting fully 3D-printed OECTs operate in the depletion mode and can be produced on flexible substrates, ensuring excellent mechanical durability and resilience in various environmental conditions. These 3D-printed OECTs exhibit impressive dopamine biosensing capabilities, detecting concentrations as low as 6 µM without the need for metal gate electrodes. Furthermore, they demonstrate long-term memory response lasting up to approximately 1 hour, highlighting their potential for diverse applications such as sensors and neuromorphic hardware. We have addressed the issue of sluggish response times in printed OECTs by utilizing multi-walled carbon nanotubes (MWCNTs) and the π-conjugated redox polymer called poly(benzimidazobenzo-phenanthroline) (BBL) to create high-performing n-type OECTs. By incorporating MWCNTs, we were able to improve the electron mobility of the transistors by more than 10 times, resulting in a rapid response time of just 15 ms and a high μC* value (which is the product of electron mobility and volumetric capacitance) of approximately 1 F cm–1 V−1 s−1. These breakthroughs have allowed us to develop complementary inverters that have a voltage gain of over 16, a significant worst-case noise margin at a supply voltage lower than 0.6 V and consume less than 1 µW of power. However, the operational stability of complementary inverters is hindered by the degradation of p-type OMIECs. The oxygen reduction reaction (ORR) is a common electrochemical side reaction that poses challenges to the stability of OECTs, but the underlying connection between ORR and material degradation remains poorly understood. In our investigation, we examined the influence of ORR on the stability and degradation mechanisms of thiophene-based OECTs. Our findings reveal that the polymer backbone experiences degradation as a result of the pH increase during ORR. To address this issue, we introduced a protective polymer glue layer between the semiconductor channel and the aqueous electrolyte, effectively suppressing the occurrence of ORR and significantly enhancing the stability of the OECTs. This improvement is evident in the nearly 90% retention of current during ≈2 hours of cycling in the saturation regime. Finally, we investigated the ionic-electronic transport properties in BBL-based OECTs using various electrolytes. We found that the peak drain current is achieved at a doping level of 1 electron per repeating unit, decreasing thereafter. The interaction between ions and the polymer reduces the voltage needed for this level of doping but also lowers the peak drain current. Unlike thiophene-based OECTs, larger cation sizes don't improve BBL-based OECT performance. Additionally, Lewis acids adversely affect BBL's electrical properties due to their impact on the polymer microstructure. We hope these studies will inspire our peers in the field of materials synthesis, device processing, and scalable digital techniques, paving the way for next-generation, reliable, and safe bioelectronics.
|
|
| 18. |
- Zhao, Dan, 1986-, et al.
(author)
-
Polymer gels with tunable ionic Seebeck coefficient for ultra-sensitive printed thermopiles
- 2019
-
In: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723 .- 2041-1723. ; 10:1
-
Journal article (peer-reviewed)abstract
- Measuring temperature and heat flux is important for regulating any physical, chemical, and biological processes. Traditional thermopiles can provide accurate and stable temperature reading but they are based on brittle inorganic materials with low Seebeck coefficient, and are difficult to manufacture over large areas. Recently, polymer electrolytes have been proposed for thermoelectric applications because of their giant ionic Seebeck coefficient, high flexibility and ease of manufacturing. However, the materials reported to date have positive Seebeck coefficients, hampering the design of ultra-sensitive ionic thermopiles. Here we report an “ambipolar” ionic polymer gel with giant negative ionic Seebeck coefficient. The latter can be tuned from negative to positive by adjusting the gel composition. We show that the ion-polymer matrix interaction is crucial to control the sign and magnitude of the ionic Seebeck coefficient. The ambipolar gel can be easily screen printed, enabling large-area device manufacturing at low cost.
|
|
