| 1. |
- Lu, Yang, et al.
(författare)
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Precise tuning of interlayer electronic coupling in layered conductive metal-organic frameworks
- 2022
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Ingår i: Nature Communications. - : Nature Portfolio. - 2041-1723. ; 13:1
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Tidskriftsartikel (refereegranskat)abstract
- Layered metal-organic frameworks attract interests for optoelectronics and spintronics. Here, the authors report a strategy to tune interlayer charge transport and thermoelectric properties via side-chain induced control of the layer spacing. Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) have attracted increasing interests for (opto)-electronics and spintronics. They generally consist of van der Waals stacked layers and exhibit layer-depended electronic properties. While considerable efforts have been made to regulate the charge transport within a layer, precise control of electronic coupling between layers has not yet been achieved. Herein, we report a strategy to precisely tune interlayer charge transport in 2D c-MOFs via side-chain induced control of the layer spacing. We design hexaiminotriindole ligands allowing programmed functionalization with tailored alkyl chains (HATI_CX, X = 1,3,4; X refers to the carbon numbers of the alkyl chains) for the synthesis of semiconducting Ni-3(HATI_CX)(2). The layer spacing of these MOFs can be precisely varied from 3.40 to 3.70 angstrom, leading to widened band gap, suppressed carrier mobilities, and significant improvement of the Seebeck coefficient. With this demonstration, we further achieve a record-high thermoelectric power factor of 68 +/- 3 nW m(-1) K-2 in Ni-3(HATI_C3)(2), superior to the reported holes-dominated MOFs.
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| 2. |
- Padinhare, Harikesh, et al.
(författare)
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Organic electrochemical neurons and synapses with ion mediated spiking
- 2022
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Ingår i: Nature Communications. - : Nature Portfolio. - 2041-1723. ; 13:1
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Tidskriftsartikel (refereegranskat)abstract
- 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. The integration of artificial neuromorphic devices with biological systems plays a fundamental role for future brain-machine interfaces, prosthetics, and intelligent soft robotics. Harikesh et al. demonstrate all-printed organic electrochemical neurons on Venus flytrap that is controlled to open and close.
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| 3. |
- Yang, Chi Yuan, et al.
(författare)
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Low-Power/High-Gain Flexible Complementary Circuits Based on Printed Organic Electrochemical Transistors
- 2022
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Ingår i: Advanced Electronic Materials. - : Wiley. - 2199-160X .- 2199-160X. ; 8:3
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Tidskriftsartikel (refereegranskat)abstract
- The ability to accurately extract low-amplitude voltage signals is crucial in several fields, ranging from single-use diagnostics and medical technology to robotics and the Internet of Things (IoT). The organic electrochemical transistor (OECT), which features large transconductance values at low operating voltages, is ideal for monitoring small signals. Here, low-power and high-gain flexible circuits based on printed complementary OECTs are reported. This work leverages the low threshold voltage of both p-type and n-type enhancement-mode OECTs to develop complementary voltage amplifiers that can sense voltages as low as 100 µV, with gains of 30.4 dB and at a power consumption of 0.1–2.7 µW (single-stage amplifier). At the optimal operating conditions, the voltage gain normalized to power consumption reaches 169 dB µW−1, which is >50 times larger than state-of-the-art OECT-based amplifiers. In a monolithically integrated two-stage configuration, these complementary voltage amplifiers reach voltage gains of 193 V/V, which are among the highest for emerging complementary metal-oxide-semiconductor-like technologies operating at supply voltages below 1 V. These flexible complementary circuits based on printed OECTs define a new power-efficient platform for sensing and amplifying low-amplitude voltage signals in several emerging beyond-silicon applications.
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| 4. |
- Zhang, Qilun, 1992-, et al.
(författare)
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Natural Product Betulin-Based Insulating Polymer Filler in Organic Solar Cells
- 2022
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Ingår i: Solar RRL. - : Wiley. - 2367-198X. ; 6:9
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Tidskriftsartikel (refereegranskat)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.
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| 5. |
- Zhang, Silan, et al.
(författare)
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Synergistic Effect of Multi-Walled Carbon Nanotubes and Ladder-Type Conjugated Polymers on the Performance of N-Type Organic Electrochemical Transistors
- 2022
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Ingår i: Advanced Functional Materials. - : Wiley. - 1616-3028 .- 1616-301X. ; 32:1
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Tidskriftsartikel (refereegranskat)abstract
- Organic electrochemical transistors (OECTs) have the potential to revolutionize the field of organic bioelectronics. To date, most of the reported OECTs include p-type (semi-)conducting polymers as the channel material, while n-type OECTs are yet at an early stage of development, with the best performing electron-transporting materials still suffering from low transconductance, low electron mobility, and slow response time. Here, the high electrical conductivity of multi-walled carbon nanotubes (MWCNTs) and the large volumetric capacitance of the ladder-type π-conjugated redox polymer poly(benzimidazobenzophenanthroline) (BBL) are leveraged to develop n-type OECTs with record-high performance. It is demonstrated that the use of MWCNTs enhances the electron mobility by more than one order of magnitude, yielding fast transistor transient response (down to 15 ms) and high μC* (electron mobility × volumetric capacitance) of about 1 F cm−1 V−1 s−1. This enables the development of complementary inverters with a voltage gain of >16 and a large worst-case noise margin at a supply voltage of <0.6 V, while consuming less than 1 µW of power.
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| 6. |
- Chen, Yongzhen, et al.
(författare)
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In Situ Spectroscopic and Electrical Investigations of Ladder-type Conjugated Polymers Doped with Alkali Metals
- 2022
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Ingår i: Macromolecules. - : American Chemical Society (ACS). - 0024-9297 .- 1520-5835. ; 55:16, s. 7294-7302
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Tidskriftsartikel (refereegranskat)abstract
- Ladder-type conjugated polymers exhibit a remarkable performance in (opto)electronic devices. Their double-stranded planar structure promotes an extended pi-conjugation compared to inter-ring-twisted analogues, providing an excellent basis for exploring the effects of charge localization on polaron formation. Here, we investigated alkali-metal n -doping of the ladder-type conjugated polymer (polybenzimidazobenzophe-nanthroline) (BBL) through detailed in situ spectroscopic and electrical characterizations. Photoelectron spectroscopy and ultraviolet-visible-near-infrared (UV-vis-NIR) spectroscopy indicate polaron formation upon potassium (K) doping, which agrees well with theoretical predictions. The semiladder BBB displays a similar evolution in the valence band with the appearance of two new features below the Fermi level upon K-doping. Compared to BBL, distinct differences appear in the UV-vis-NIR spectra due to more localized polaronic states in BBB. The high conductivity (2 S cm(-1)) and low activation energy (44 meV) measured for K-doped BBL suggest disorder-free polaron transport. An even higher conductivity (37 S cm(-1)) is obtained by changing the dopant from K to lithium (Li). We attribute the enhanced conductivity to a decreased perturbation of the polymer nanostructure induced by the smaller Li ions. These results highlight the importance of polymer chain planarity and dopant size for the polaronic state in conjugated polymers.
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| 7. |
- Wu, Hanyan, et al.
(författare)
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Influence of Molecular Weight on the Organic Electrochemical Transistor Performance of Ladder-Type Conjugated Polymers
- 2022
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Ingår i: Advanced Materials. - : Wiley-V C H Verlag GMBH. - 0935-9648 .- 1521-4095. ; 34:4
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Tidskriftsartikel (refereegranskat)abstract
- 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 (g(m,norm) approximate to 11 S cm(-1)) and electron mobility x volumetric capacitance (mu C* approximate to 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.
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| 8. |
- Xu, Kai, et al.
(författare)
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On the Origin of Seebeck Coefficient Inversion in Highly Doped Conducting Polymers
- 2022
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Ingår i: Advanced Functional Materials. - : Wiley-V C H Verlag GMBH. - 1616-301X .- 1616-3028. ; 32:20
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Tidskriftsartikel (refereegranskat)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.
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