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1.
ACS Appl Mater Interfaces ; 12(5): 6144-6150, 2020 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-31918540

RESUMO

The molecular structure of polymer electrets is crucial for creating diverse functionalities of organic field-effect transistor (OFET) devices. Herein, a conceptual framework has been applied in this study to design the highly photoresponsive carbazole-based copolymer electret materials for the application of photoresponsive OFET memory. As an electret layer, two 1,8-carbazole-based copolymers were utilized; the copoly(CT) consisted of carbazole as the donor group and thiophene as the π-spacer, whereas the copoly(CBT) was further introduced as an acceptor moiety, benzothiadiazole, for comparison. Both copolymers exhibited efficient visible-light absorption and photoluminescence quenching in the film state, indicating the formation of a considerable number of nonemissive excitons, one of the crucial factors for achieving photoinduced recovery behavior in OFET memories. Compared to copoly(CT) with the pure donor system, faster and more effective photoinduced recovery behavior was discovered in the copoly(CBT) with the conjugated donor-acceptor structure because of the coexistence of the conjugated donor and acceptor groups. Thus, the dissociation of the generated excitons facilitated the stimulating of the unique ambipolar trapping property, resulting in the high-density data storage devices with multilevel current states. In addition, the nonvolatile and durable characteristics demonstrated the feasibility in application of memory and photorecorders.

2.
Nat Commun ; 11(1): 387, 2020 Jan 20.
Artigo em Inglês | MEDLINE | ID: mdl-31959755

RESUMO

Miniaturized photonic sources based on semiconducting two-dimensional (2D) materials offer new technological opportunities beyond the modern III-V platforms. For example, the quantum-confined 2D electronic structure aligns the exciton transition dipole moment parallel to the surface plane, thereby outcoupling more light to air which gives rise to high-efficiency quantum optics and electroluminescent devices. It requires scalable materials and processes to create the decoupled multi-quantum-well superlattices, in which individual 2D material layers are isolated by atomically thin quantum barriers. Here, we report decoupled multi-quantum-well superlattices comprised of the colloidal quantum wells of lead halide perovskites, with unprecedentedly ultrathin quantum barriers that screen interlayer interactions within the range of 6.5 Å. Crystallographic and 2D k-space spectroscopic analysis reveals that the transition dipole moment orientation of bright excitons in the superlattices is predominantly in-plane and independent of stacking layer and quantum barrier thickness, confirming interlayer decoupling.

3.
J Synchrotron Radiat ; 27(Pt 1): 217-221, 2020 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-31868755

RESUMO

Time-resolved X-ray excited optical luminescence (TR-XEOL) was developed successfully for the 23A X-ray nanoprobe beamline located at the Taiwan Photon Source (TPS). The advantages of the TR-XEOL facility include (i) a nano-focused X-ray beam (<60 nm) with excellent spatial resolution and (ii) a streak camera that can simultaneously record the XEOL spectrum and decay time. Three time spans, including normal (30 ps to 2 ns), hybrid (30 ps to 310 ns) and single (30 ps to 1.72 µs) bunch modes, are available at the TPS, which can fulfil different experimental conditions involving samples with various lifetimes. It is anticipated that TR-XEOL at the TPS X-ray nanoprobe could provide great characterization capabilities for investigating the dynamics of photonic materials.

4.
Macromol Rapid Commun ; 41(3): e1900542, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-31880040

RESUMO

A compatible organic/inorganic nanocomposite film for a stretchable resistive memory device with high performance is demonstrated using poly(4-vinylpyridine)-block-poly(propyl methacrylate) (P4VP-b-PPMA) with zinc oxide (ZnO) nanoparticle. The PPMA soft segment is designed for reducing the rigidity of the active layer, while the P4VP block serves as a charge-trapping component to induce conductive filament and also a compatible moiety for inorganic nanoparticles through hydrogen bonding. The experimental results show that the P4VP-b-PPMA-based electrical memory device exhibits write-once-read-many-times memory behavior and an excellent ON/OFF current ratio of over 105 with a stable turn-on voltage (Vset ) around -2.0 V and stable memory behavior upon stretching up to 60% strain. On the other hand, P4VP-b-PPMA/ZnO nanocomposite film switches the memory characteristic to the dynamic random access memory behavior. The stretchable memory device prepared from the nanocomposite film can have a stretching durability over 40% strain and up to 1000 times cycling stretch-relaxation test. This work demonstrates a new strategy using nanocomposite films with tunable electrical characteristics and enhanced mechanical properties for stretchable electrical devices.

5.
ACS Appl Mater Interfaces ; 11(13): 12723-12732, 2019 Apr 03.
Artigo em Inglês | MEDLINE | ID: mdl-30854843

RESUMO

A new strategy for influencing the solid-state morphology of conjugated polymers was developed through physical blending with a low-molecular-weight branched polyethylene. This nontoxic and low-boiling-point additive was blended with a high-charge-mobility diketopyrrolopyrrole-based conjugated polymer, and a detailed investigation of the new blended materials was performed by various characterization tools, including X-ray diffraction, UV-vis spectroscopy, and atomic force microscopy. Interestingly, the branched additive was shown to reduce the crystallinity of the conjugated polymer while promoting aggregation and phase separation in the solid state. Upon thermal removal of the olefinic additive, the thin films maintained a lower crystallinity and aggregated morphology in comparison to a nonblended polymer. The semiconducting performance of the new branched polyethylene/conjugated polymer blends was also investigated in organic field-effect transistors, which showed a stable charge mobility of around 0.3 cm2 V-1 s-1 without thermal annealing, independent of the blending ratio. Furthermore, using the new polyethylene-based additive, the concentration of a conjugated polymer required for the fabrication of organic field-effect transistor devices was reduced down to 0.05 wt %, without affecting charge transport, which represents a significant improvement compared to usual concentrations used for solution deposition. Our results demonstrate that the physical blending of a conjugated polymer with nontoxic, low-molecular-weight branched polyethylene is a promising strategy for the modification and fine-tuning of the solid-state morphology of conjugated polymers without sacrificing their charge-transport properties, thus creating new opportunities for the large-scale processing of organic semiconductors.

6.
Exp Clin Transplant ; 17(6): 838-840, 2019 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-30373507

RESUMO

Drug-drug interactions between azoles and calcineurin inhibitors can cause issues for organ transplant specialists. Clinical practice guidelines for the treatment of solid-organ transplant recipients with invasive aspergillosis infection are lacking. Here, we present a patient who developed pulmonary aspergillosis after liver transplant. The patient had prolonged treatment with echinocandin that was not effective. A drug-drug interaction between azoles and tacrolimus caused issues for the clinical physician. We adjusted the doses, and the patient was successfully treated. A reduction in the tacrolimus dose, intensive monitoring of associated parameters, and elimination of risk exposures are important for a favorable outcome.

7.
Small ; 14(51): e1804006, 2018 12.
Artigo em Inglês | MEDLINE | ID: mdl-30394008

RESUMO

Enabling mechanical responsiveness in field-effect transistors (FETs) offers new technological opportunity beyond the reach of existing platforms. Here a new force-sensing concept is proposed by controlling the wettability of a semiconductor surface, referring to the interfacial field-effect transistors (IFETs). An IFET made by superhydrophobic semiconductor nanowires (NWs) sandwiched between a layer of 2D electron gas (2DEG) and a conductive Cassie-Baxter (CB) sessile droplet is designed. Following the hydrostatic deformation of the CB droplet upon mechanical stress, an extremely small elastic modulus of 820 pascals vertical to the substrate plane, or ≈100 times softer than Ecoflex rubbers, enabling an excellent stress detection limit down to <10 pascals and a stress sensitivity of 36 kPa-1 is proposed. The IFET exhibits an on/off current ratio exceeding 3 × 104 , as the carrier density profile at the NW/2DEG interface is modulated by a partially penetrated electrostatic field. This study demonstrates a versatile platform that bridges multiple macroscopic interfacial phenomena with nanoelectronic responses.

8.
Sci Adv ; 3(12): eaaq0208, 2017 12.
Artigo em Inglês | MEDLINE | ID: mdl-29282451

RESUMO

The outstanding excitonic properties, including photoluminescence quantum yield (ηPL), of individual, quantum-confined semiconductor nanoparticles are often significantly quenched upon aggregation, representing the main obstacle toward scalable photonic devices. We report aggregation-induced emission phenomena in lamellar solids containing layer-controlled colloidal quantum wells (QWs) of hybrid organic-inorganic lead bromide perovskites, resulting in anomalously high solid-state ηPL of up to 94%. Upon forming the QW solids, we observe an inverse correlation between exciton lifetime and ηPL, distinct from that in typical quantum dot solid systems. Our multiscale theoretical analysis reveals that, in a lamellar solid, the collective motion of the surface organic cations is more restricted to orient along the [100] direction, thereby inducing a more direct bandgap that facilitates radiative recombination. Using the QW solids, we demonstrate ultrapure green emission by completely downconverting a blue gallium nitride light-emitting diode at room temperature, with a luminous efficacy higher than 90 lumen W-1 at 5000 cd m-2, which has never been reached in any nanomaterial assemblies by far.

9.
Nano Lett ; 17(9): 5277-5284, 2017 09 13.
Artigo em Inglês | MEDLINE | ID: mdl-28770603

RESUMO

Pure green light-emitting diodes (LEDs) are essential for realizing an ultrawide color gamut in next-generation displays, as is defined by the recommendation (Rec.) 2020 standard. However, because the human eye is more sensitive to the green spectral region, it is not yet possible to achieve an ultrapure green electroluminescence (EL) with a sufficiently narrow bandwidth that covers >95% of the Rec. 2020 standard in the CIE 1931 color space. Here, we demonstrate efficient, ultrapure green EL based on the colloidal two-dimensional (2D) formamidinium lead bromide (FAPbBr3) hybrid perovskites. Through the dielectric quantum well (DQW) engineering, the quantum-confined 2D FAPbBr3 perovskites exhibit a high exciton binding energy of 162 meV, resulting in a high photoluminescence quantum yield (PLQY) of ∼92% in the spin-coated films. Our optimized LED devices show a maximum current efficiency (ηCE) of 13.02 cd A-1 and the CIE 1931 color coordinates of (0.168, 0.773). The color gamut covers 97% and 99% of the Rec. 2020 standard in the CIE 1931 and the CIE 1976 color space, respectively, representing the "greenest" LEDs ever reported. Moreover, the device shows only a ∼10% roll-off in ηCE (11.3 cd A-1) at 1000 cd m-2. We further demonstrate large-area (3 cm2) and ultraflexible (bending radius of 2 mm) LEDs based on 2D perovskites.

10.
Adv Mater ; 29(33)2017 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-28640532

RESUMO

Solution-processable organic-inorganic hybrid perovskite materials with a wealth of exotic semiconducting properties have appeared as the promising front-runners for next-generation electronic devices. Further, regarding its well photoresponsibility, various perovskite-based photosensing devices are prosperously developed in recent years. However, most exploited devices to date only transiently transduce the optical signals into electrical circuits while under illumination, which necessitates using additional converters to further store the output signals for recording the occurrence of light stimulation. Herein, a nonvolatile perovskite-based floating-gate photomemory with a multilevel memory behavior is demonstrated, for which a floating gate comprising a polymer matrix impregnated with perovskite nanoparticles is employed. Owing to the well photoresponsibility introduced by the embedded nanoparticles, the device is enabled to access multiple wavelength response and the functionalities of recording power/time-dependent illumination under no vertical electrical field. Intriguingly, a nonvolatility of photorecording exceeding three months with a high On/Off current ratio over 104 can be achieved.

11.
Nature ; 539(7629): 411-415, 2016 11 17.
Artigo em Inglês | MEDLINE | ID: mdl-27853213

RESUMO

Thin-film field-effect transistors are essential elements of stretchable electronic devices for wearable electronics. All of the materials and components of such transistors need to be stretchable and mechanically robust. Although there has been recent progress towards stretchable conductors, the realization of stretchable semiconductors has focused mainly on strain-accommodating engineering of materials, or blending of nanofibres or nanowires into elastomers. An alternative approach relies on using semiconductors that are intrinsically stretchable, so that they can be fabricated using standard processing methods. Molecular stretchability can be enhanced when conjugated polymers, containing modified side-chains and segmented backbones, are infused with more flexible molecular building blocks. Here we present a design concept for stretchable semiconducting polymers, which involves introducing chemical moieties to promote dynamic non-covalent crosslinking of the conjugated polymers. These non-covalent crosslinking moieties are able to undergo an energy dissipation mechanism through breakage of bonds when strain is applied, while retaining high charge transport abilities. As a result, our polymer is able to recover its high field-effect mobility performance (more than 1 square centimetre per volt per second) even after a hundred cycles at 100 per cent applied strain. Organic thin-film field-effect transistors fabricated from these materials exhibited mobility as high as 1.3 square centimetres per volt per second and a high on/off current ratio exceeding a million. The field-effect mobility remained as high as 1.12 square centimetres per volt per second at 100 per cent strain along the direction perpendicular to the strain. The field-effect mobility of damaged devices can be almost fully recovered after a solvent and thermal healing treatment. Finally, we successfully fabricated a skin-inspired stretchable organic transistor operating under deformations that might be expected in a wearable device.


Assuntos
Materiais Biomiméticos/química , Biomimética , Polímeros/química , Transistores Eletrônicos , Humanos , Maleabilidade , Pele , Estresse Mecânico , Cicatrização
12.
ACS Nano ; 10(10): 9720-9729, 2016 Oct 25.
Artigo em Inglês | MEDLINE | ID: mdl-27684448

RESUMO

Solution-processed hybrid organic-inorganic lead halide perovskites are emerging as one of the most promising candidates for low-cost light-emitting diodes (LEDs). However, due to a small exciton binding energy, it is not yet possible to achieve an efficient electroluminescence within the blue wavelength region at room temperature, as is necessary for full-spectrum light sources. Here, we demonstrate efficient blue LEDs based on the colloidal, quantum-confined 2D perovskites, with precisely controlled stacking down to one-unit-cell thickness (n = 1). A variety of low-k organic host compounds are used to disperse the 2D perovskites, effectively creating a matrix of the dielectric quantum wells, which significantly boosts the exciton binding energy by the dielectric confinement effect. Through the Förster resonance energy transfer, the excitons down-convert and recombine radiatively in the 2D perovskites. We report room-temperature pure green (n = 7-10), sky blue (n = 5), pure blue (n = 3), and deep blue (n = 1) electroluminescence, with record-high external quantum efficiencies in the green-to-blue wavelength region.

13.
J Am Chem Soc ; 138(18): 6020-7, 2016 05 11.
Artigo em Inglês | MEDLINE | ID: mdl-27099162

RESUMO

A self-healing dielectric elastomer is achieved by the incorporation of metal-ligand coordination as cross-linking sites in nonpolar polydimethylsiloxane (PDMS) polymers. The ligand is 2,2'-bipyridine-5,5'-dicarboxylic amide, while the metal salts investigated here are Fe(2+) and Zn(2+) with various counteranions. The kinetically labile coordination between Zn(2+) and bipyridine endows the polymer fast self-healing ability at ambient condition. When integrated into organic field-effect transistors (OFETs) as gate dielectrics, transistors with FeCl2 and ZnCl2 salts cross-linked PDMS exhibited increased dielectric constants compared to PDMS and demonstrated hysteresis-free transfer characteristics, owing to the low ion conductivity in PDMS and the strong columbic interaction between metal cations and the small Cl(-) anions which can prevent mobile anions drifting under gate bias. Fully stretchable transistors with FeCl2-PDMS dielectrics were fabricated and exhibited ideal transfer characteristics. The gate leakage current remained low even after 1000 cycles at 100% strain. The mechanical robustness and stable electrical performance proved its suitability for applications in stretchable electronics. On the other hand, transistors with gate dielectrics containing large-sized anions (BF4(-), ClO4(-), CF3SO3(-)) displayed prominent hysteresis due to mobile anions drifting under gate bias voltage. This work provides insights on future design of self-healing stretchable dielectric materials based on metal-ligand cross-linked polymers.


Assuntos
Metais/química , Polímeros/química , 2,2'-Dipiridil , Cloretos/química , Reagentes para Ligações Cruzadas , Dimetilpolisiloxanos/química , Elasticidade , Eletrônica , Compostos Ferrosos/química , Ligantes , Compostos de Zinco/química
14.
Sci Rep ; 6: 20129, 2016 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-26831222

RESUMO

UNLABELLED: Nano-floating gate memory devices (NFGM) using metal nanoparticles (NPs) covered with an insulating polymer have been considered as a promising electronic device for the next-generation nonvolatile organic memory applications NPs. However, the transparency of the device with metal NPs is restricted to 60~70% due to the light absorption in the visible region caused by the surface plasmon resonance effects of metal NPs. To address this issue, we demonstrate a novel NFGM using the blends of hole-trapping poly (9-(4-vinylphenyl) carbazole) (PVPK) and electron-trapping ZnO NPs as the charge storage element. The memory devices exhibited a remarkably programmable memory window up to 60 V during the program/erase operations, which was attributed to the trapping/detrapping of charge carriers in ZnO NPs/PVPK composite. Furthermore, the devices showed the long-term retention time (>10(5) s) and WRER test (>200 cycles), indicating excellent electrical reliability and stability. Additionally, the fabricated transistor memory devices exhibited a relatively high transparency of 90% at the wavelength of 500 nm based on the spray-coated PEDOT: PSS as electrode, suggesting high potential for transparent organic electronic memory devices.

15.
Nano Lett ; 15(11): 7587-95, 2015 Nov 11.
Artigo em Inglês | MEDLINE | ID: mdl-26496513

RESUMO

Due to the lack of a bandgap, applications of graphene require special device structures and engineering strategies to enable semiconducting characteristics at room temperature. To this end, graphene-based vertical field-effect transistors (VFETs) are emerging as one of the most promising candidates. Previous work attributed the current modulation primarily to gate-modulated graphene-semiconductor Schottky barrier. Here, we report the first experimental evidence that the partially screened field effect and selective carrier injection through graphene dominate the electronic transport at the organic semiconductor/graphene heterointerface. The new mechanistic insight allows us to rationally design graphene VFETs. Flexible organic/graphene VFETs with bending radius <1 mm and the output current per unit layout area equivalent to that of the best oxide planar FETs can be achieved. We suggest driving organic light emitting diodes with such VFETs as a promising application.

16.
Adv Mater ; 27(40): 6257-64, 2015 Oct 28.
Artigo em Inglês | MEDLINE | ID: mdl-26332569

RESUMO

Oligosaccharides are one of the most promising biomaterials because they are abundant, renewable, diversified, and biosourced. The use of oligo- or polysaccharides for high-performance non-volatile organic field-effect-transistor memory is demonstrated herein. The charge-storage mechanism is attributed to charged hydroxyl groups that induce stronger hydrogen bonding, thus leading to the stabilization of trapped charges. This study reveals a promising future for green memory devices.

17.
ACS Appl Mater Interfaces ; 6(15): 12780-8, 2014 Aug 13.
Artigo em Inglês | MEDLINE | ID: mdl-24998629

RESUMO

Organic nonvolatile transistor memory devices of the n-type semiconductor N,N'-bis(2-phenylethyl)-perylene-3,4:9,10-tetracarboxylic diimide (BPE-PTCDI) were prepared using various electrets (i.e., three-armed star-shaped poly[4-(diphenylamino)benzyl methacrylate] (N(PTPMA)3) and its blends with 6,6-phenyl-C61-butyric acid methyl ester (PCBM), 6,13-bis(triisopropylsilylethynyl)pentacene (TIPS-pen) or ferrocene). In the device using the PCBM:N(PTPMA)3 blend electret, it changed its memory feature from a write-once-read-many (WORM) type to a flash type as the PCBM content increased and could be operated repeatedly based on a tunneling process. The large shifts on the reversible transfer curves and the hysteresis after implementing a gate bias indicated the considerable charge storage in the electret layer. On the other hand, the memory characteristics showed a flash type and a WORM characteristic, respectively, using the donor/donor electrets TIPS-pen:N(PTPMA)3 and ferrocene:N(PTPMA)3. The variation on the memory characteristics was attributed to the difference of energy barrier at the interface when different types of electret materials were employed. All the studied memory devices exhibited a long retention over 10(4) s with a highly stable read-out current. In addition, the afore-discussed memory devices by inserting another electret layer of poly(methacrylic acid) (PMAA) between the BPE-PTCDI layer and the semiconducting blend layer enhanced the write-read-erase-read (WRER) operation cycle as high as 200 times. This study suggested that the energy level and charge transfer in the blend electret had a significant effect on tuning the characteristics of nonvolatile transistor memory devices.

18.
Macromol Rapid Commun ; 35(11): 1039-45, 2014 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-24700508

RESUMO

The electrical memory characteristics of the n-channel organic field-effect transistors (OFETs) employing diverse polyimide (PI) electrets are reported. The synthesized PIs comprise identical electron donor and three different building blocks with gradually increasing electron-accepting ability. The distinct charge-transfer capabilities of these PIs result in varied type of memory behaviors from the write-one-read-many (WORM) to flash type. Finally, a prominent flexible WORM-type transistor memory is demonstrated and shows not only promising write-many-read-many (WMRM) multilevel data storage but also excellent mechanical and retention stability.


Assuntos
Resinas Sintéticas/química , Transistores Eletrônicos , Técnicas Eletroquímicas , Teoria Quântica , Resinas Sintéticas/síntese química , Dióxido de Silício/química
19.
ACS Appl Mater Interfaces ; 6(8): 5506-15, 2014 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-24673527

RESUMO

In this work, a single electrospun polymer nanofiber was employed as an additional dielectric in organic field-effect transistors where the active channel was a layer of pentacene. A high field-effect mobility (>1.50 cm(2)/(V·s)) and a high ON/OFF current ratio (>10(6)) could be achieved by the use of such a nanofiber. Probing by electron microscopy, atomic force microscopy, and scattering techniques, we found that the geometry of the fiber is key to induce a pentacene morphology with large and oriented grains that facilitates the charge transport in pentacene layer along the fiber. The feasibility of nonvolatile memory based on this new type of transistor has been explored and the devices showed a fairly high memory window and reliable memory characteristics. In addition to pure polymers, the effects of composite nanofibers with dispersed [6,6]-phenyl-C61-butyric acid methyl ester were also investigated, and the electrical properties and memory characteristics of the transistors were found to be further improved. This study highlights the importance of dielectric geometry to pentacene morphology that is decisive for the performances of organic field-effect transistors.

20.
Chem Commun (Camb) ; 50(24): 3217-9, 2014 Mar 25.
Artigo em Inglês | MEDLINE | ID: mdl-24522655

RESUMO

Solution-processable nonvolatile transistor memory devices on a flexible ITO-PEN substrate are demonstrated using the charge storage dielectrics of poly(methacrylic acid) and graphene oxide (PMAA-GO) composites. The hydrogen bonding interaction effectively disperses GO sheets in the high-k PMAA matrix, leading to the control on the memory characteristics. Besides, the fabricated transistor memory devices have a low operation voltage, a large threshold voltage shift of 5.3-9.4 V, a long retention ability of up to 10(4) s, and good stress endurance of at least 100 cycles.

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