Organic electrochemical transistors (OECTs) hold promise for developing a variety of high‐performance (bio‐)electronic devices/circuits. While OECTs based on p‐type semiconductors have achieved ...tremendous progress in recent years, n‐type OECTs still suffer from low performance, hampering the development of power‐efficient electronics. Here, it is demonstrated that fine‐tuning the molecular weight of the rigid, ladder‐type n‐type polymer poly(benzimidazobenzophenanthroline) (BBL) by only one order of magnitude (from 4.9 to 51 kDa) enables the development of n‐type OECTs with record‐high geometry‐normalized transconductance (gm,norm ≈ 11 S cm−1) and electron mobility × volumetric capacitance (µC* ≈ 26 F cm−1 V−1 s−1), fast temporal response (0.38 ms), and low threshold voltage (0.15 V). This enhancement in OECT performance is ascribed to a more efficient intermolecular charge transport in high‐molecular‐weight BBL than in the low‐molecular‐weight counterpart. OECT‐based complementary inverters are also demonstrated with record‐high voltage gains of up to 100 V V−1 and ultralow power consumption down to 0.32 nW, depending on the supply voltage. These devices are among the best sub‐1 V complementary inverters reported to date. These findings demonstrate the importance of molecular weight in optimizing the OECT performance of rigid organic mixed ionic–electronic conductors and open for a new generation of power‐efficient organic (bio‐)electronic devices.
n‐Type organic electrochemical transistors (OECTs) underperform compared to p‐type OECTs. By tuning the molecular weight of the rigid ladder‐type poly(benzimidazobenzophenanthroline), n‐type OECTs with record‐high figures of merit are reported. OECT‐based complementary inverters are also demonstrated with high voltage gains of up to 100 V V−1 and ultralow power consumption down to 0.32 nW, depending on the supply voltage.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Conjugated polymers with high thermoelectric performance enable the fabrication of low‐cost, large‐area, low‐toxicity, and highly flexible thermoelectric devices. However, compared to their p‐type ...counterparts, n‐type polymer thermoelectric materials show much lower performance, which is largely due to inefficient doping and a much lower conductivity. Herein, it is reported that the development of a donor–acceptor (D–A) polymer with enhanced n‐doping efficiency through donor engineering of the polymer backbone. Both a high n‐type electrical conductivity of 1.30 S cm−1 and an excellent power factor (PF) of 4.65 µW mK−2 are obtained, which are the highest reported values among D–A polymers. The results of multiple characterization techniques indicate that electron‐withdrawing modification of the donor units enhances the electron affinity of the polymer and changes the polymer packing orientation, leading to substantially improved miscibility and n‐doping efficiency. Unlike previous studies in which improving the polymer‐dopant miscibility typically resulted in lower mobilities, the strategy maintains the mobility of the polymer. All these factors lead to prominent enhancement of three orders magnitude in both the electrical conductivity and the PF compared to those of the non‐engineered polymer. The results demonstrate that proper donor engineering can enhance the n‐doping efficiency, electrical conductivity, and thermoelectric performance of D–A copolymers.
1000‐fold enhancements in n‐type electrical conductivity and power factor of a donor–acceptor copolymer are obtained by donor engineering. Donor engineering enhances electron affinity and n‐doping efficiency, prevents phase separation, lowers hopping barrier and keeps mobility unaffected. A record electrical conductivity of 1.30 S cm−1 and a power factor of 4.65 μW mK−2 are achieved in this work.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Future brain-machine interfaces, prosthetics, and intelligent soft robotics will require integrating artificial neuromorphic devices with biological systems. Due to their poor biocompatibility, ...circuit complexity, low energy efficiency, and operating principles fundamentally different from the ion signal modulation of biology, traditional Silicon-based neuromorphic implementations have limited bio-integration potential. Here, we report the first organic electrochemical neurons (OECNs) with ion-modulated spiking, based on all-printed complementary organic electrochemical transistors. We demonstrate facile bio-integration of OECNs with Venus Flytrap (Dionaea muscipula) to induce lobe closure upon input stimuli. The OECNs can also be integrated with all-printed organic electrochemical synapses (OECSs), exhibiting short-term plasticity with paired-pulse facilitation and long-term plasticity with retention >1000 s, facilitating Hebbian learning. These soft and flexible OECNs operate below 0.6 V and respond to multiple stimuli, defining a new vista for localized artificial neuronal systems possible to integrate with bio-signaling systems of plants, invertebrates, and vertebrates.
Conducting polymers, such as the p-doped poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS), have enabled the development of an array of opto- and bio-electronics devices. However, ...to make these technologies truly pervasive, stable and easily processable, n-doped conducting polymers are also needed. Despite major efforts, no n-type equivalents to the benchmark PEDOT:PSS exist to date. Here, we report on the development of poly(benzimidazobenzophenanthroline):poly(ethyleneimine) (BBL:PEI) as an ethanol-based n-type conductive ink. BBL:PEI thin films yield an n-type electrical conductivity reaching 8 S cm
, along with excellent thermal, ambient, and solvent stability. This printable n-type mixed ion-electron conductor has several technological implications for realizing high-performance organic electronic devices, as demonstrated for organic thermoelectric generators with record high power output and n-type organic electrochemical transistors with a unique depletion mode of operation. BBL:PEI inks hold promise for the development of next-generation bioelectronics and wearable devices, in particular targeting novel functionality, efficiency, and power performance.
Abstract
Objective
To mine Twitter and quantitatively analyze COVID-19 symptoms self-reported by users, compare symptom distributions across studies, and create a symptom lexicon for future research.
...Materials and Methods
We retrieved tweets using COVID-19-related keywords, and performed semiautomatic filtering to curate self-reports of positive-tested users. We extracted COVID-19-related symptoms mentioned by the users, mapped them to standard concept IDs in the Unified Medical Language System, and compared the distributions to those reported in early studies from clinical settings.
Results
We identified 203 positive-tested users who reported 1002 symptoms using 668 unique expressions. The most frequently-reported symptoms were fever/pyrexia (66.1%), cough (57.9%), body ache/pain (42.7%), fatigue (42.1%), headache (37.4%), and dyspnea (36.3%) amongst users who reported at least 1 symptom. Mild symptoms, such as anosmia (28.7%) and ageusia (28.1%), were frequently reported on Twitter, but not in clinical studies.
Conclusion
The spectrum of COVID-19 symptoms identified from Twitter may complement those identified in clinical settings.
Abstract
N-doping plays an irreplaceable role in controlling the electron concentration of organic semiconductors thus to improve performance of organic semiconductor devices. However, compared with ...many mature p-doping methods, n-doping of organic semiconductor is still of challenges. In particular, dopant stability/processability, counterion-semiconductor immiscibility and doping induced microstructure non-uniformity have restricted the application of n-doping in high-performance devices. Here, we report a computer-assisted screening approach to rationally design of a triaminomethane-type dopant, which exhibit extremely high stability and strong hydride donating property due to its thermally activated doping mechanism. This triaminomethane derivative shows excellent counterion-semiconductor miscibility (counter cations stay with the polymer side chains), high doping efficiency and uniformity. By using triaminomethane, we realize a record n-type conductivity of up to 21 S cm
−1
and power factors as high as 51 μW m
−1
K
−2
even in films with thicknesses over 10 μm, and we demonstrate the first reported all-polymer thermoelectric generator.
Molecular doping is a powerful method to fine‐tune the thermoelectric properties of organic semiconductors, in particular to impart the requisite electrical conductivity. The incorporation of ...molecular dopants can, however, perturb the microstructure of semicrystalline organic semiconductors, which complicates the development of a detailed understanding of structure–property relationships. To better understand how the doping pathway and the resulting dopant counterion influence the thermoelectric performance and transport properties, a new dimer dopant, (N‐DMBI)2, is developed. Subsequently, FBDPPV is then n‐doped with dimer dopants (N‐DMBI)2, (RuCp*mes)2, and the hydride‐donor dopant N‐DMBI‐H. By comparing the UV–vis–NIR absorption spectra and morphological characteristics of the doped polymers, it is found that not only the doping mechanism, but also the shape of the counterion strongly influence the thermoelectric properties and transport characteristics. (N‐DMBI)2, which is a direct electron‐donating dopant with a comparatively small, relatively planar counterion, gives the best power factor among the three systems studied here. Additionally, temperature‐dependent conductivity and Seebeck coefficient measurements differ between the three dopants with (N‐DMBI)2 yielding the best thermoelectric properties. The results of this study of dopant effects on thermoelectric properties provide insight into guidelines for future organic thermoelectrics.
A novel dimeric n‐dopant (N‐DMBI)2, is designed and synthesized to understand the effects of molecular dopants on thermoelectric properties. This study shows how the counterion shape, and the doping mechanism affect the thermoelectric performance and the transport pathway of n‐type conducting polymers, and reveals what type of n‐dopant is preferable.
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FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Doping of organic semiconductors is crucial for the operation of organic (opto)electronic and electrochemical devices. Typically, this is achieved by adding heterogeneous dopant molecules to the ...polymer bulk, often resulting in poor stability and performance due to dopant sublimation or aggregation. In small-molecule donor-acceptor systems, charge transfer can yield high and stable electrical conductivities, an approach not yet explored in all-conjugated polymer systems. Here, we report ground-state electron transfer in all-polymer donor-acceptor heterojunctions. Combining low-ionization-energy polymers with high-electron-affinity counterparts yields conducting interfaces with resistivity values five to six orders of magnitude lower than the separate single-layer polymers. The large decrease in resistivity originates from two parallel quasi-two-dimensional electron and hole distributions reaching a concentration of ∼10
cm
. Furthermore, we transfer the concept to three-dimensional bulk heterojunctions, displaying exceptional thermal stability due to the absence of molecular dopants. Our findings hold promise for electro-active composites of potential use in, for example, thermoelectrics and wearable electronics.
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FZAB, GEOZS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
Organic field‐effect transistors (OFETs) with impressively high hole mobilities over 10 cm2 V−1 s−1 and electron mobilities over 1 cm2 V−1 s−1 have been reported in the past few years. However, ...significant non‐ideal electrical characteristics, e.g., voltage‐dependent mobilities, have been widely observed in both small‐molecule and polymer systems. This issue makes the accurate evaluation of the electrical performance impossible and also limits the practical applications of OFETs. Here, a semiconductor‐unrelated, charge‐trapping‐induced non‐ideality in OFETs is reported, and a revised model for the non‐ideal transfer characteristics is provided. The trapping process can be directly observed using scanning Kelvin probe microscopy. It is found that such trapping‐induced non‐ideality exists in OFETs with different types of charge carriers (p‐type or n‐type), different types of dielectric materials (inorganic and organic) that contain different functional groups (OH, NH2, COOH, etc.). As fas as it is known, this is the first report for the non‐ideal transport behaviors in OFETs caused by semiconductor‐independent charge trapping. This work reveals the significant role of dielectric charge trapping in the non‐ideal transistor characteristics and also provides guidelines for device engineering toward ideal OFETs.
A mechanism of non‐ideal behavior in organic field‐effect transistors (OFETs) is reported. This mechanism is general for various p‐ and n‐type small‐molecule and polymer transistors with different types of dielectrics (inorganic and organic) that contain different functional groups. This work provides a new insight into the fundamental aspects of non‐ideality, and also guidelines for device engineering toward ideal OFETs.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Polymer self‐assembly in solution prior to film fabrication makes solution‐state structures critical for their solid‐state packing and optoelectronic properties. However, unraveling the ...solution‐state supramolecular structures is challenging, not to mention establishing a clear relationship between the solution‐state structure and the charge‐transport properties in field‐effect transistors. Here, for the first time, it is revealed that the thin‐film morphology of a conjugated polymer inherits the features of its solution‐state supramolecular structures. A “solution‐state supramolecular structure control” strategy is proposed to increase the electron mobility of a benzodifurandione‐based oligo(p‐phenylene vinylene) (BDOPV)‐based polymer. It is shown that the solution‐state structures of the BDOPV‐based conjugated polymer can be tuned such that it forms a 1D rod‐like structure in good solvent and a 2D lamellar structure in poor solvent. By tuning the solution‐state structure, films with high crystallinity and good interdomain connectivity are obtained. The electron mobility significantly increases from the original value of 1.8 to 3.2 cm2 V−1 s−1. This work demonstrates that “solution‐state supramolecular structure” control is critical for understanding and optimization of the thin‐film morphology and charge‐transport properties of conjugated polymers.
A supramolecular self‐assembly strategy is used to control the solution‐state structure of a conjugated polymer. It is revealed that the thin‐film morphology of the conjugated polymer inherits the features of their solution‐state supramolecular structures. Through “solution‐state supramolecular structure control”, the electron mobility of the polymer is boosted to 3.2 cm2 V−1 s−1, nearly doubling the original performance.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
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