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1.
Cell ; 180(2): 311-322.e15, 2020 01 23.
Artigo em Inglês | MEDLINE | ID: mdl-31883793

RESUMO

The propagation of electrical impulses along axons is highly accelerated by the myelin sheath and produces saltating or "jumping" action potentials across internodes, from one node of Ranvier to the next. The underlying electrical circuit, as well as the existence and role of submyelin conduction in saltatory conduction remain, however, elusive. Here, we made patch-clamp and high-speed voltage-calibrated optical recordings of potentials across the nodal and internodal axolemma of myelinated neocortical pyramidal axons combined with electron microscopy and experimentally constrained cable modeling. Our results reveal a nanoscale yet conductive periaxonal space, incompletely sealed at the paranodes, which separates the potentials across the low-capacitance myelin sheath and internodal axolemma. The emerging double-cable model reproduces the recorded evolution of voltage waveforms across nodes and internodes, including rapid nodal potentials traveling in advance of attenuated waves in the internodal axolemma, revealing a mechanism for saltation across time and space.


Assuntos
Potenciais de Ação/fisiologia , Bainha de Mielina/fisiologia , Fibras Nervosas Mielinizadas/fisiologia , Nós Neurofibrosos/fisiologia , Animais , Axônios/metabolismo , Axônios/fisiologia , Masculino , Modelos Neurológicos , Fibras Nervosas Mielinizadas/metabolismo , Técnicas de Patch-Clamp/métodos , Células Piramidais/fisiologia , Ratos , Ratos Wistar
2.
Angew Chem Int Ed Engl ; 61(35): e202209316, 2022 Aug 26.
Artigo em Inglês | MEDLINE | ID: mdl-35785422

RESUMO

Double-cable conjugated polymers with near-infrared (NIR) electron acceptors are synthesized for use in single-component organic solar cells (SCOSCs). Through the development of a judicious synthetic pathway, the highly sensitive nature of the 2-(3-oxo-2,3-dihydroinden-1-ylidene)malononitrile (IC)-based electron acceptors in basic and protonic solvents is overcome. In addition, an asymmetric design motif is adopted to optimize the packing of donor and acceptor segments, enhancing charge separation efficiency. As such, the new double-cable polymers are successfully applied in SCOSCs, providing an efficiency of over 10 % with a broad photo response from 300 to 850 nm and exhibiting excellent thermal/light stability. These results demonstrate the powerful design of NIR-acceptor-based double-cable polymers and will enable SCOSCs to enter a new stage.

3.
Angew Chem Int Ed Engl ; 60(48): 25499-25507, 2021 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-34546627

RESUMO

We developed a series of highly crystalline double-cable conjugated polymers for application in single-component organic solar cells (SCOSCs). These polymers contain conjugated backbones as electron donor and pendant perylene bisimide units (PBIs) as electron acceptor. PBIs are connected to the backbone via alkyl units varying from hexyl (C6 H12 ) to eicosyl (C20 H40 ) as flexible linkers. For double-cable polymers with short linkers, the PBIs tend to stack in a head-to-head fashion, resulting in large d-spacings (e.g. 64 Šfor the polymer P12 with C12 H24 linker) along the lamellar stacking direction. When the length of the linker groups is longer than a certain length, the PBIs instead adopt a more ordered packing likely via H-aggregation, resulting in short d-spacings (e.g. 50 Šfor the polymer P16 with C16 H32 linker). This work highlights the importance of linker length on the molecular packing of the acceptor units and the influences on the photovoltaic performance of SCOSCs.

4.
Angew Chem Int Ed Engl ; 59(48): 21683-21692, 2020 Nov 23.
Artigo em Inglês | MEDLINE | ID: mdl-32815586

RESUMO

A record power conversion efficiency of 8.40 % was obtained in single-component organic solar cells (SCOSCs) based on double-cable conjugated polymers. This is realized based on exciton separation playing the same role as charge transport in SCOSCs. Two double-cable conjugated polymers were designed with almost identical conjugated backbones and electron-withdrawing side units, but extra Cl atoms had different positions on the conjugated backbones. When Cl atoms were positioned at the main chains, the polymer formed the twist backbones, enabling better miscibility with the naphthalene diimide side units. This improves the interface contact between conjugated backbones and side units, resulting in efficient conversion of excitons into free charges. These findings reveal the importance of charge generation process in SCOSCs and suggest a strategy to improve this process: controlling miscibility between conjugated backbones and aromatic side units in double-cable conjugated polymers.

5.
Angew Chem Int Ed Engl ; 58(43): 15532-15540, 2019 Oct 21.
Artigo em Inglês | MEDLINE | ID: mdl-31469224

RESUMO

The crystalline cooperativity of the donor and acceptor segment in double-cable conjugated polymers plays an important role in the nanophase separation and photovoltaic performance in single-component organic solar cells (SCOSCs). Two double-cable conjugated polymers with the same conjugated backbone and perylene bisimide (PBI) side units were designed in which PBIs were positioned symmetrically and perpendicularly (P1) and asymmetrically and slantingly (P2) along the conjugated backbones. After thermal annealing, both conjugated backbones and PBI side units in P1 tend to form ordered nanostructures, while PBI side units in P2 dominated the crystallization and hamper the crystallization of conjugated backbones. P1 showed good crystalline cooperativity between conjugated backbones and PBI side units, resulting in improved power conversion efficiencies (PCEs) up to 3.43 % in SCOSCs, while P2 with poor crystalline cooperativity exhibited PCEs below 2.42 %.

6.
Chemistry ; 23(5): 1018-1022, 2017 Jan 23.
Artigo em Inglês | MEDLINE | ID: mdl-27689679

RESUMO

Hexasubstituted C3 -symmetric benzenes with three elongated shape-persistent oligo(phenylenevinylene) arms and three pyridyl hydrogen-bond acceptors have been synthesized. These mesogens assemble in a double-helical columnar liquid crystal (LC) structure, owing to the compensation of free spaces between conjugated arms by dimer formation. The void is filled also by up to three anthracene carboxylic acids as guests forming hydrogen bonded supermesogens assembling in columnar LC and soft-crystal phases. Thin film fluorescence and solid-state NMR spectroscopy imply a transition from a disordered columnar LC to an unexpected double nanosegregated morphology of a filled soft columnar crystal phase. An additional intracolumnar separation of anthracene and oligo(phenylenevinylene) chromophores occurs, separate to the general segregation of aliphatic and aromatic building blocks in LC structures. The new type of supermesogens will enable the rational design of host-guest double cables with a wide range of different conjugated building blocks.

7.
Adv Mater ; : e2409212, 2024 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-39194393

RESUMO

Single-component organic solar cells based on double cable polymers have achieved remarkable performance, with DCPY2 reaching a high efficiency of over 13%. In this study, DCPY2 is further optimized with an efficiency of 13.85%, maintaining a high fill factor (FF) without compromising the short circuit current. Despite its intermixed morphology, DCPY2 shows a reduced recombination rate compared to their binary counterpart (PBDB-T:Y-O6). This slower recombination in DCPY2 is attributed to the reduced wavefunction overlap of delocalized charges, achieved by spatially separating the donor and acceptor units with an alkyl linker, thereby restricting the recombination pathways. Adding 1,8-diiodooctane (DIO) into DCPY2 further reduced the recombination rate by facilitating acceptor aggregation, allowing free charges to become more delocalized. The DIO-assisted aggregation in DCPY2 (5% DIO) is evidenced by an increased pseudo-pure domain size of Y-O6. Fine molecular control at the donor/acceptor interface in the double-cable polymer achieves reduced non-geminate recombination under efficient charge generation, increased mobility, and charge carrier lifetime, thereby achieving superior performance. Nevertheless, the FF is still limited by relatively low mobility compared to the blend, suggesting the potential for further mobility improvement through enhanced higher-dimensional packing of the double-cable material.

8.
ACS Appl Mater Interfaces ; 15(37): 44054-44061, 2023 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-37694683

RESUMO

The invention of near-infrared pedant-based double-cable conjugated polymers has demonstrated remarkable efficacy in single-component organic solar cells (SCOSCs). This work focuses on the innovative double-cable conjugated polymers aimed at attaining good absorption and suitable energy levels. Specifically, in the aromatic side units, the electron-donating (D) part is designed using a thieno[3,4-c]pyrrole-4,6-dione (TPD) as a core unit, flanked by two cyclopentadithiophene groups on either side. The electron-deficient (A) terminal groups consist of 2-(3-oxo-2,3-dihydro-1H-cyclopenta[b]naphthalen-1-ylidene) malononitrile (NC), which can be further modified through fluorination to modulate the physical properties and packing modes of the acceptor material. The resulting double-cable conjugated polymers exhibit broad absorption spectra spanning 500-850 nm and possess lowered Frontier energy levels when incorporating fluorine elements, providing decreased voltage losses in SCOSCs. Therefore, SCOSCs fabricated using these polymers have demonstrated power conversion efficiencies ranging from 7.6 to 10.2%, in which fluorine-containing double-cable conjugated polymers showed higher PCEs due to more favorable crystalline packing, enhanced exciton dissociation probability, and charge-transporting ability.

9.
Adv Mater ; 35(18): e2300629, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36814317

RESUMO

Double-cable conjugated polymers with pendent electron acceptors, including fullerene, rylene diimides, and nonfused acceptors, have been developed for application in single-component organic solar cells (SCOSCs) with efficiencies approaching 10%. In this work, Y-series electron acceptors have been firstly incorporated into double-cable polymers in order to further improve the efficiencies of SCOSCs. A highly crystalline Y-series acceptor based on quinoxaline core and the random copolymerized strategy are used to optimize the ambipolar charge transport and the nanophase separation of the double-cable polymers. As a result, an efficiency of 13.02% is obtained in the random double-cable polymer, representing the highest performance in SCOSCs, while the regular double-cable polymer only provides a low efficiency of 2.75%. The significantly enhanced efficiencies are attributed to higher charge carrier mobilities, better ordering conjugated backbones and Y-series acceptors in random double-cable polymers.

10.
ACS Appl Mater Interfaces ; 14(42): 47952-47960, 2022 Oct 26.
Artigo em Inglês | MEDLINE | ID: mdl-36222398

RESUMO

In this work, we have introduced single/double-sided N-annulated perylene bisimide (PBI) with deep energy levels into double-cable polymers with poly[1-(5-(4,8-bis(4-chloro-5-(2-ethylhexyl)thiophen-2-yl)-6-methylbenzo[1,2-b:4,5-b']dithiophen-2-yl)thiophen-2-yl)-5,7-bis(2-ethylhexyl)-3-(5-methylthiophen-2-yl)-4H,8H-benzo[1,2-c:4,5-c']dithiophene-4,8-dione] (PBDB-T-Cl) as a donor backbone, marking as s-PPNR and as-PPNR, according to the molecular symmetry. Both double-cable polymers displayed a high open-circuit voltage approaching 1.20 V in light of high energy level discrepancy between electron-donating and electron-withdrawing parts, which is the highest open-circuit voltage among double-cable-based single-component organic solar cell (SCOSC) devices. Additionally, the asymmetric polymer displayed improved absorption spectra, thereby promoting crystallization and phase separation. Consequently, the as-PPNR-based SCOSCs achieved a power conversion efficiency of 5.05% along with a higher short-circuit current density and fill factor than their s-PPNR-based counterparts. In this work, we have successfully incorporated N-annulated PBI into double-cable polymers and revealed the important effects on structural symmetry and phase separation of double-cable polymers for higher SCOSC performance.

11.
Polymers (Basel) ; 13(10)2021 May 18.
Artigo em Inglês | MEDLINE | ID: mdl-34070205

RESUMO

A new side-chain C60-fullerene functionalized thiophene copolymer bearing tributylphosphine-substituted hexylic lateral groups was successfully synthesized by means of a fast and effective post-polymerization reaction on a regioregular ω-alkylbrominated polymeric precursor. The growth of the polymeric intermediate was followed by NMR spectrometry in order to determine the most convenient reaction time. The obtained copolymer was soluble in water and polar solvents and was used as a photoactive layer in single-material organic photovoltaic (OPV) solar cells. The copolymer photovoltaic efficiency was compared with that of an OPV cell containing a water-soluble polythiophenic homopolymer, functionalized with the same tributylphosphine-substituted hexylic side chains, in a blend with a water-soluble C60-fullerene derivative. The use of a water-soluble double-cable copolymer made it possible to enhance the control on the nanomorphology of the active blend, thus reducing phase-segregation phenomena, as well as the macroscale separation between the electron acceptor and donor components. Indeed, the power conversion efficiency of OPV cells based on a single material was higher than that obtained with the classical architecture, involving the presence of two distinct ED and EA materials (PCE: 3.11% vs. 2.29%, respectively). Moreover, the synthetic procedure adopted to obtain single material-based cells is more straightforward and easier than that used for the preparation of the homopolymer-based BHJ solar cell, thus making it possible to completely avoid the long synthetic pathway which is required to prepare water-soluble fullerene derivatives.

12.
Small Methods ; 5(9): e2100481, 2021 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-34928045

RESUMO

Owing to the advantages of being lightweight and compatible with surfaces with different deformations, flexible organic solar cells (OSCs) have broad scopes of applications, including wearable electronics and portable devices. Most flexible OSCs focus on the two-component bulk-heterojunction (BHJ) photo-active layers, but they usually suffer from degradation problems both in efficiency and mechanical durability derived from the limited phase stability under mechanical and thermal stress. Whereas, single-component organic solar cells (SCOSCs) based on the double-cable conjugated polymer are supposed to possess excellent mechanical robustness and long-term stability. Here, the first flexible SCOSCs based on a double-cable polymer are fabricated on a transparent silver nanowires (AgNWs) electrode on a plastic foil. Impressively, the obtained flexible SCOSCs exhibited a power conversion efficiency (PCE) of 7.21%. The flexible SCOSCs are further demonstrated to possess superior mechanical robustness (>95% retention after 1000 bending cycles) and storage stability (>97% retention after 430 h in nitrogen atmosphere) compared to several BHJ-type flexible OSCs. The pseudo-free-standing tensile test and morphology investigation are conducted to reveal the distinction in mechanical durability of the single-component polymer film and the BHJ-type films. Besides, ultraflexible SCOSCs are also fabricated, indicating the application prospect and superiority in flexible devices and wearable electronic products.

13.
ACS Appl Mater Interfaces ; 12(7): 8826-8834, 2020 Feb 19.
Artigo em Inglês | MEDLINE | ID: mdl-31984740

RESUMO

Double-cable conjugated polymers and two-dimensional (2D) perovskites are both promising materials for next-generation photodetectors (PDs) due to their solution processibility and tunable optoelectronic properties. In this work, a lateral PD is designed by layering a double-cable conjugated polymer film atop a 2D Ruddlesden-Popper perovskite film. Compared to the corresponding single-layer polymer and perovskite PDs, the heterojunction device exhibits greatly improved performance with a high responsivity of 27.06 A W-1, an on/off ratio of 1379, and a short rise/decay time of 3.53/3.78 ms. In addition, a flexible device using polyimide as the substrate is successfully fabricated and exhibits comparable performance with the device on glass. This work demonstrates the great potential of double-cable polymer/2D perovskite heterojunctions in future flexible optoelectronics.

14.
Front Neurosci ; 11: 250, 2017.
Artigo em Inglês | MEDLINE | ID: mdl-28559787

RESUMO

Tactile sensory feedback plays an important role in our daily life. Transcutaneous electrical nerve stimulation (TENS) is widely accepted to produce artificial tactile sensation. To explore the underlying mechanism of tactile sensation under TENS, this paper presented a novel 3D TENS computational model including an active Aß tactile nerve fiber (TNF) model and a forearm finite element model with the fine-layered skin structure. The conduction velocity vs. fiber diameter and strength-duration relationships in this combined TENS model matched well with experimental data. Based on this validated TENS model, threshold current variation were further investigated under different stimulating electrode sizes with varied fiber diameters. The computational results showed that the threshold current intensity increased with electrode size, and larger nerve fibers were recruited at lower current intensities. These results were comparable to our psychophysical experimental data from six healthy subjects. This novel 3D TENS model would further guide the floorplan of the surface electrodes, and the stimulating paradigms for tactile sensory feedback.

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