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1.
Angew Chem Int Ed Engl ; : e202403068, 2024 Apr 30.
Artículo en Inglés | MEDLINE | ID: mdl-38687308

RESUMEN

Organic self-assembled molecules (OSAMs) based hole transporting materials play a pivotal role in achieving highly efficient and stable inverted perovskite solar cells (IPSCs). However, the reported carbazol-based OSAMs have serious drawbacks, such as poor solubility in alcohol solution, worse matched energy arrangement with perovskite, and limited molecular species, which greatly limit the device performance. To address above problems, a novel OSAM 4-(3,6-glycol monomethyl ether-9H-carbazol-9-yl) butyl]phosphonic acid (GM-4PACz) was synthesized as hole-transporting material by introducing glycol monomethyl ether (GM) side chains at carbazolyl unit. GM groups enhance the surface energy of Indium Tin Oxide (ITO)/SAM substrate to facilitate the nucleation and growth of up perovskite film, suppress cation defects, release the residual stress at SAM/perovskite interface, and evaluate energy level for matching with perovskite. Consequently, the GM-4PACz based IPSC achieves a champion PCE of 25.52%, a respectable open-circuit voltage (VOC) of 1.21 V, a high stability, possessing 93.29% and 91.75% of their initial efficiency after aging in air for 2000 h or tracking at maximum power point for 1000 h, respectively.

2.
ACS Appl Mater Interfaces ; 16(10): 12897-12906, 2024 Mar 13.
Artículo en Inglés | MEDLINE | ID: mdl-38412379

RESUMEN

The "von Neumann bottleneck" is a formidable challenge in conventional computing, driving exploration into artificial synapses. Organic semiconductor materials show promise but are hindered by issues such as poor adhesion and a high elastic modulus. Here, we combine polyisoindigo-bithiophene (PIID-2T) with grafted poly(dimethylsiloxane) (PDMS) to synthesize the triblock-conjugated polymer (PIID-2T-PDMS). The polymer exhibited substantial enhancements in adhesion (4.8-68.8 nN) and reductions in elastic modulus (1.6-0.58 GPa) while maintaining the electrical characteristics of PIID-2T. The three-terminal organic synaptic transistor (three-terminal p-type organic artificial synapse (TPOAS)), constructed using PIID-2T-PDMS, exhibits an unprecedented analog switching range of 276×, surpassing previous records, and a remarkable memory on-off ratio of 106. Moreover, the device displays outstanding operational stability, retaining 99.6% of its original current after 1600 write-read events in the air. Notably, TPOAS replicates key biological synaptic behaviors, including paired-pulse facilitation (PPF), short-term plasticity (STP), and long-term plasticity (LTP). Simulations using handwritten digital data sets reveal an impressive recognition accuracy of 91.7%. This study presents a polyisoindigo-bithiophene-based block copolymer that offers enhanced adhesion, reduced elastic modulus, and high-performance artificial synapses, paving the way for the next generation of neuromorphic computing systems.

3.
Angew Chem Int Ed Engl ; 63(5): e202315537, 2024 Jan 25.
Artículo en Inglés | MEDLINE | ID: mdl-38081781

RESUMEN

The ion/chemical-based modulation feature of organic mixed ionic-electronic conductors (OMIECs) are critical to advancing next generation bio-integrated neuromorphic hardware. Despite achievements with polymeric OMIECs in organic electrochemical neuronal synapse (OENS). However, small molecule OMIECs based OENS has not yet been realized. Here, for the first time, we demonstrate an effective materials design concept of combining n-type fused all-acceptor small molecule OMIECs with subtle side chain optimization that enables robustly and flexibly modulating versatile synaptic behavior and sensing neurotransmitter in solid or aqueous electrolyte, operating in accumulation modes. By judicious tuning the ending side chains, the linear oligoether and butyl chain derivative gNR-Bu exhibits higher recognition accuracy for a model artificial neural network (ANN) simulation, higher steady conductance states and more outstanding ambient stability, which is superior to the state-of-art n-type OMIECs based OENS. These superior artificial synapse characteristics of gNR-Bu can be attributed to its higher crystallinity with stronger ion bonding capacities. More impressively, we unprecedentedly realized n-type small-molecule OMIECs based OENS as a neuromorphic biosensor enabling to respond synaptic communication signals of dopamine even at sub-µM level in aqueous electrolyte. This work may open a new path of small-molecule ion-electron conductors for next-generation ANN and bioelectronics.

4.
ACS Nano ; 17(21): 21935-21946, 2023 11 14.
Artículo en Inglés | MEDLINE | ID: mdl-37922489

RESUMEN

Noninvasive testing and continuous monitoring of ultralow-concentration hormones in biofluids have attracted increasing interest for health management and personalized medicine, in which saliva could fulfill the demand. Steroid sex hormones such as progesterone (P4) and ß-estradiol (E2) are crucial for female wellness and reproduction; however, their concentrations in saliva can vary down to sub-pM and constantly fluctuate over several orders of magnitude. This remains a major obstacle toward user-friendly and reliable monitoring at home with low-cost flexible biosensors. Herein we introduce a 3D micropyramidal electrode architecture to address such challenges and achieve an ultrasensitive flexible electrochemical immunosensor with sub-fM-level detection capability of salivary sex hormones within a few minutes. This is enabled by micropyramidal electrode arrays consisting of a poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate) (PEDOT:PSS) thin film as the coating layer and electrochemically decorated gold nanoparticles (AuNPs) to improve the antibody immobilization. The enhanced mass transport around the 3D tips provided by the micropyramidal architecture is discovered to improve the detection limit by 3 orders of magnitude, pushing it to as low as ∼100 aM for P4 and ∼20 aM for E2, along with a wide linear range up to µM. Accordingly, these hormones down to sub-fM in >1000-fold-diluted saliva samples can be accurately measured by the printed soft immunosensors, thus allowing at-home testing through simple saliva dilution to minimize the interfering substances instead of centrifugation. Finally, monitoring of the female ovarian hormone cycle of both P4 and E2 is successfully demonstrated based on the centrifuge-free saliva testing during a period of 4 weeks. This ultrasensitive and soft 3D microarchitected electrode design is believed to provide a universal platform for a diverse variety of applications spanning from accurate clinical diagnostics and counselling and in vivo detection of bioactive species to environmental and food quality tracing.


Asunto(s)
Técnicas Biosensibles , Nanopartículas del Metal , Femenino , Humanos , Nanopartículas del Metal/química , Oro/química , Inmunoensayo , Polímeros/química , Electrodos , Hormonas Esteroides Gonadales , Esteroides , Hormonas , Técnicas Electroquímicas
5.
Appl Opt ; 62(27): 7233-7239, 2023 Sep 20.
Artículo en Inglés | MEDLINE | ID: mdl-37855579

RESUMEN

Phase sensitive amplifiers (PSAs) based on optical parametric amplification feature near noiseless amplification, which is of considerable benefit for improving the performance of optical communication systems. Currently, the majority of research on PSAs is carried out on the basis of highly nonlinear fibers or periodically poled lithium niobite waveguides, with the impediments of being susceptible to environmental interference and requiring complex temperature control systems to maintain quasi-phase matching conditions, respectively. Here, a near-noiseless and small-footprint PSA based on dispersion-engineered AlGaAs-on-insulator (AlGaAsOI) waveguides is proposed and demonstrated theoretically. The phase-dependent gain and the phase-to-phase transfer function of the PSA are calculated to analyze its characteristics. Furthermore, we investigate in detail the effects of linear loss, nonlinear coefficient, and pump power on the PSA gain and noise figure (NF) in AlGaAsOI waveguides. The results show that a PSA based on an AlGaAsOI waveguide is feasible with a maximum phase sensitive gain of 33 dB, achieving an NF of less than 1 dB over a gain bandwidth of 245 nm with a gain of >15d B, which completely covers the S + C + L band. This investigation is worthwhile for noiseless PSAs on photonic integrated chips, which are promising for low-noise optical amplification, multifunctional photonic integrated chips, quantum communication, and spectroscopy, and as a reference for low-noise PSAs depending on the third-order nonlinearity, χ (3), of the waveguide material.

6.
Opt Express ; 31(17): 27433-27449, 2023 Aug 14.
Artículo en Inglés | MEDLINE | ID: mdl-37710819

RESUMEN

The utilization of mid-infrared (mid-IR) light spanning the 3-5 µm range presents notable merits over the 1.5 µm band when operating in adverse atmospheric conditions. Consequently, it emerges as a promising prospect for serving as optical carriers in free-space communication (FSO) through atmospheric channels. However, due to the insufficient performance level of devices in the mid-IR band, the capability of mid-IR communication is hindered in terms of transmission capacity and signal format. In this study, we conduct experimental investigations on the transmission of time-domain multiplexed ultra-short optical pulse streams, with a pulse width of 1.8 ps and a data rate of up to 40 Gbps at 3.6 µm, based on the difference frequency generation (DFG) effect. The mid-IR transmitter realizes an effective wavelength conversion of optical time division multiplexing (OTDM) signals from 1.5 µm to 3.6 µm, and the obtained power of the 40 Gbps mid-IR OTDM signal at the optimum temperature of 54.8 °C is 7.4 dBm. The mid-IR receiver successfully achieves the regeneration of the 40 Gbps 1.5 µm OTDM signal, and the corresponding regenerated power at the optimum temperature of 51.5 °C is -30.56 dBm. Detailed results pertaining to the demodulation of regeneration 1.5 µm OTDM signal have been acquired, encompassing parameters such as pulse waveform diagram, bit error rate (BER), and Q factor. The estimated power penalty of the 40 Gbps mid-IR OTDM transmission is 2.4 dB at a BER of 1E-6, compared with the back-to-back (BTB) transmission. Moreover, it is feasible by using chirped PPLN crystals with wider bandwidth to increase the data rate to the order of one hundred gigabits.

7.
ACS Appl Mater Interfaces ; 15(35): 41656-41665, 2023 Sep 06.
Artículo en Inglés | MEDLINE | ID: mdl-37610705

RESUMEN

Organic electrochemical transistors (OECTs) for skin-like bioelectronics require mechanical stretchability, softness, and cost-effective large-scale manufacturing. However, developing intrinsically stretchable OECTs using a simple and fast-response technique is challenging due to limitations in functional materials, substrate wettability, and integrated processing of multiple materials. In this regard, we propose a fabrication method devised by combining the preparation of a microstructured hydrophilic substrate, multi-material printing of functional inks with varying viscosities, and optimization of the device channel geometries. The resulting intrinsically stretchable OECT array with synaptic properties was successfully manufactured. These devices demonstrated high transconductance (22.5 mS), excellent mechanical softness (Young's modulus ∼ 2.2 MPa), and stretchability (∼30%). Notably, the device also exhibited artificial synapse functionality, mimicking the biological synapse with features such as paired-pulse depression, short-term plasticity, and long-term plasticity. This study showcases a promising strategy for fabricating intrinsically stretchable OECTs and provides valuable insights for the development of brain-computer interfaces.

8.
Opt Express ; 31(9): 15156-15169, 2023 Apr 24.
Artículo en Inglés | MEDLINE | ID: mdl-37157363

RESUMEN

The 3∼5 µm mid-infrared (mid-IR) light has several exceptional benefits in the case of adverse atmospheric conditions compared to the 1.5 µm band, so it is a promising candidate for optical carriers for free-space communication (FSO) through atmospheric channels. However, the transmission capacity in the mid-IR band is constrained in the lower range due to the immaturity of its devices. In this work, to replicate the 1.5 µm band dense wavelength division multiplexing (DWDM) technology to the 3 µm band for high-capacity transmission, we demonstrate a 12-channel 150 Gbps FSO transmission in the 3 µm band based on our developed mid-IR transmitter and receiver modules. These modules enable wavelength conversion between the 1.5 µm and 3 µm bands based on the effect of difference-frequency generation (DFG). The mid-IR transmitter effectively generates up to 12 optical channels ranging from 3.5768 µm to 3.5885 µm with a power of 6.6 dBm, and each channel carries 12.5 Gbps binary phase shift keying (BPSK) modulated data. The mid-IR receiver regenerates the 1.5 µm band DWDM signal with a power of -32.1 dBm. Relevant results of regenerated signal demodulation have been collected in detail, including bit error ratio (BER), constellation diagram, and eye diagram. The power penalties of the 6th to 8th channels selected from the regenerated signal are lower than 2.2 dB compared with back-to-back (BTB) DWDM signal at a bit error ratio (BER) of 1E-6, and other channels can also achieve good transmission quality. It is expected to further push the data capacity to the terabit-per-second level by adding more 1.5 µm band laser sources and using wider-bandwidth chirped nonlinear crystals.

9.
Opt Express ; 30(18): 32306-32316, 2022 Aug 29.
Artículo en Inglés | MEDLINE | ID: mdl-36242295

RESUMEN

In recent years, the thriving satellite laser communication industry has been severely hindered by the limitations of incompatible modulation formats and restricted Size Weight and Power (SWaP). A multi-modulation compatible method serving for free-space optical (FSO) communication has been proposed assisted by chirp-managed laser (CML). The corresponding demonstration system has been established for realizing free-switching between intensity (OOK) and phase modulation (RZ-DPSK). The feasibility and performance of system have been evaluated sufficiently when loading with 2.5 and 5 Gbps data streams, respectively. Additionally, a control-group system has been operated utilizing Mach-Zehnder modulator (MZM) for comparison between CML-based and MZM-based compatibility solutions. The OOK receiving sensitivities of CML-based system are -47.02 dBm@2.5 Gbps and -46.12 dBm@5 Gbps at BER of 1×10-3 which are 0.62 dB and 1.11 dB higher than that of MZM; the receiving sensitivities of RZ-DPSK are -50.12 dBm@2.5 Gbps and -47.03 dBm@5 Gbps which are 0.79 dB and 0.47 dB higher than that of MZM respectively. Meanwhile, CML-based transmitter abandoned the traditional modulator and its complicated supporting devices which can effectively contribute to the reduction of SWaP. The CML-based system has been proven to have the compatibility between intensity and phase modulation while also possesses a miniaturized design. It may provide fresh thinking to achieve a practical miniaturization system for satisfying the requirements of space optical network in future.

10.
Opt Express ; 30(20): 35300-35310, 2022 Sep 26.
Artículo en Inglés | MEDLINE | ID: mdl-36258484

RESUMEN

A high-sensitivity and large-capacity free space optical (FSO) communication scheme based on the soliton microcomb (SMC) is proposed. Using ultra-large bandwidth stabilized SMC with a frequency interval of 48.97 GHz as the laser source, 60 optical wavelengths modulated by 2.5 Gbit/s 16-Pulse position modulation (PPM) are transmitted in parallel. A corresponding outfield high-sensitivity 150 Gbit/s FSO communication experiment based on the SMC was carried out with 1 km space distance. Our experimental results show that the best sensitivity of the single comb wavelength which has higher OSNR can reach -52.62 dBm, and the difference is only 1.38 dB from the theoretical limit under the BER of 1 × 10-3 without forward error correction (FEC). In addition, at BER of 1 × 10-3, 16-PPM has a higher received sensitivity of 6.73dB and 3.72dB compared to on-off keying (OOK) and differential phase shift keying (DPSK) respectively. Meanwhile, taking the advantage of multi-channel SMC, 60 × 2.5 Gbit/s can achieve 150 Gbit/s large-capacity free-space transmission. For comparison, commercially available single-wavelength laser based FSO communication system have also been performed in the outfield. The outfield experimental results demonstrated the feasibility of high-sensitivity, large-capacity PPM FSO communication based on SMCs and provided a new perspective for the future development of large-capacity, long-haul FSO communication.

11.
Nanomicro Lett ; 14(1): 184, 2022 Sep 12.
Artículo en Inglés | MEDLINE | ID: mdl-36094765

RESUMEN

Organic electrochemical transistors (OECTs) have emerged as versatile platforms for broad applications spanning from flexible and wearable integrated circuits to biomedical monitoring to neuromorphic computing. A variety of materials and tailored micro/nanostructures have recently been developed to realized stretchable OECTs, however, a solid-state OECT with high elasticity has not been demonstrated to date. Herein, we present a general platform developed for the facile generation of highly elastic all-polymer OECTs with high transconductance (up to 12.7 mS), long-term mechanical and environmental durability, and sustainability. Rapid prototyping of these devices was achieved simply by transfer printing lithium bis(trifluoromethane)sulfonimide doped poly(3,4-ethylenedioxythiophene): poly(styrene sulfonate) (PEDOT:PSS/LiTFSI) microstructures onto a resilient gelatin-based gel electrolyte, in which both depletion-mode and enhancement-mode OECTs were produced using various active channels. Remarkably, the elaborate 3D architectures of the PEDOT:PSS were engineered, and an imprinted 3D-microstructured channel/electrolyte interface combined with wrinkled electrodes provided performance that was retained (> 70%) through biaxial stretching of 100% strain and after 1000 repeated cycles of 80% strain. Furthermore, the anti-drying and degradable gelatin and the self-crosslinked PEDOT:PSS/LiTFSI jointly enabled stability during > 4 months of storage and on-demand disposal and recycling. This work thus represents a straightforward approach towards high-performance stretchable organic electronics for wearable/implantable/neuromorphic/sustainable applications.

12.
Animals (Basel) ; 12(12)2022 Jun 13.
Artículo en Inglés | MEDLINE | ID: mdl-35739867

RESUMEN

Betaine is a well-established supplement used in livestock feeding. In our previous study, betaine was shown to result in the redistribution of body fat, a healthier steatosis phenotype, and an increased liver weight and triglyceride storage of the Landes goose liver, which is used for foie-gras production. However, these effects are not found in other species and strains, and the underlying mechanism is unclear. Here, we studied the underpinning molecular mechanisms by developing an in vitro fatty liver cell model using primary Landes goose hepatocytes and a high-glucose culture medium. Oil red-O staining, a mitochondrial membrane potential assay, and a qRT-PCR were used to quantify lipid droplet characteristics, mitochondrial ß-oxidation, and fatty acid metabolism-related gene expression, respectively. Our in vitro model successfully simulated steatosis caused by overfeeding. Betaine supplementation resulted in small, well-distributed lipid droplets, consistent with previous experiments in vivo. In addition, mitochondrial membrane potential was restored, and gene expression of fatty acid synthesis genes (e.g., sterol regulatory-element binding protein, diacylglycerol acyltransferase 1 and 2) was lower after betaine supplementation. By contrast, the expression of lipid hydrolysis transfer genes (mitochondrial transfer protein and lipoprotein lipase) was higher. Overall, the results provide a scientific basis and theoretical support for the use of betaine in animal production.

13.
Nanoscale ; 14(18): 7055-7074, 2022 May 16.
Artículo en Inglés | MEDLINE | ID: mdl-35475488

RESUMEN

Water pollution control is one of the major challenges currently faced. With the development of photocatalytic technology, an increasing number of new and efficient catalysts have been developed, but most of the catalysts have limited light capture ability and catalytic degradation efficiency. Therefore, in this work, hydrogen peroxide was further introduced to establish a photo-Fenton system to improve the photocatalytic effect by constructing a Z-scheme, and the degradation ability of the catalyst was maximized. Moreover, we successfully adhered bismuth tungstate nanosheets onto the surface of a MIL-101(Fe) framework and changed the number of active sites with iron ions of different doping amounts. We found that the number of active sites in the photo-Fenton system does not increase linearly, but increases and decreases regularly, which is similar to the change in band structure after doping. In addition, the results of the radical scavenger experiment and electron paramagnetic resonance (EPR) revealed that both hydroxide radical (˙OH) and superoxide radical (˙O2-) participated in methylene blue (MB) degradation, of which ˙OH was the main active species for pollutant degradation. Based on high-performance liquid chromatography-mass spectrometry (HPLC-MS) analysis, the possible degradation pathways were proposed. We believed that this work will provide insights into the heterojunction photo-Fenton system.

14.
J Colloid Interface Sci ; 616: 858-871, 2022 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-35257935

RESUMEN

The development of the effective diagnostic method for the determination of cancer biomarkers is one of the most promising strategies for early clinical diagnosis of cancer. Here, based on the preparation of heterogeneous cuprous oxide coated silver (Ag@Cu2O) nanocomposites/graphitic carbon nitride (g-C3N4)/cadmium sulfide (CdS) nanoarrays structure, a highly sensitive photoelectrochemical (PEC) biosensor for the examination of carcinoembryonic antigen (CEA) has been constructed successfully. The combination of photoactive semiconductor materials g-C3N4 and CdS increases the electron transfer rate between them and enhances their photocurrent response, thus greatly increasing the concentration detection range. At the same time, the specific recognition between antigen and antibody is used to form a sandwich structure secondary antibody (Ab2)/CEA/antibody (Ab1). And because Ag@Cu2O has the function of absorbing light and consuming electron donor. Therefore, the successful measurement of CEA was achieved by labeling Ag@Cu2O on Ab2 and finally immobilizing it on the sensor to correlate the current reduction with the CEA concentration. The sandwich PEC biosensor proposed by this signal amplification strategy under optimal conditions has good analytical performance for CEA, with a wide linear detection range (from 10-5 to 1 ng/mL) and a low detection limit of 0.0011 pg/mL. The PEC biosensor constructed by this method showed high sensitivity, excellent anti-interference ability, favourable repeatability, and good stability.


Asunto(s)
Técnicas Biosensibles , Nanocompuestos , Cadmio , Compuestos de Cadmio , Antígeno Carcinoembrionario , Cobre , Técnicas Electroquímicas/métodos , Grafito , Inmunoensayo/métodos , Límite de Detección , Nanocompuestos/química , Compuestos de Nitrógeno , Plata , Sulfuros
15.
ACS Appl Mater Interfaces ; 14(10): 12583-12595, 2022 Mar 16.
Artículo en Inglés | MEDLINE | ID: mdl-35230799

RESUMEN

Hydrogel electrolytes as soft ionic conductors have been extensively exploited to establish skinlike and biocompatible devices. However, in many common hydrogels, there exists irreversible elongation upon prolonged stretching cycles and poor interfacial contact, which have significantly hindered their practical applications where long-term operation at large deformations is needed. Herein, multifunctional soft electronic devices with reversible stretchability and improved electrode/electrolyte interfaces are demonstrated by employing polyacrylamide-based double-network organohydrogel electrolytes soaked with a high content of tannic acid (TA) that affords multiple noncovalent interactions and redox activity. Performances of the TA-rich gels are evaluated for the first time in realizing shape-recoverable stretchable devices against repeated deformations to 500% strain, with superior gel-electrode interfaces exhibiting both intimate adhesion and boosted electrochemical capacitance of >200 mF·cm-2. A maximal 4-fold higher capacitance can be achieved by introducing TA and ethylene glycol (EG) into hydrogels. Moreover, a soft electronic system consisting of stretchable supercapacitors and gel-based microsensors was demonstrated, in which the electronic performance of these devices can be well preserved after >1000 repeated cycles at strains of up to 200%, without obvious residual strain or electrode delamination. This could pave a route to the design of multifunctional gel networks tackling both the mechanical and interfacial issues in soft and biocompatible devices.

16.
ACS Appl Mater Interfaces ; 13(19): 22757-22764, 2021 May 19.
Artículo en Inglés | MEDLINE | ID: mdl-33973469

RESUMEN

Mid-infrared (MIR) photodetection is of significance in civil and military applications because it shows superiority in absorbing the vibration of various molecules and covering atmospheric transmission windows. Recently, the PtTe2, a typical type-II Dirac semimetal, has come under the spotlight due to its unique photodetection sensibility in the MIR region and robust stability in the atmosphere. Here, the high-quality and large-scale 1T-PtTe2 thin films with air stability were grown by molecular beam epitaxy. Broadband photoresponse of the photodetectors of PtTe2 from 420 nm to 10.7 µm shows high responsivity and detectivity of 0.2 mA W-1 and 2.6 × 107 Jones at 10.7 µm and 1.6 mA W-1 and 2.2 × 108 Jones at 4.7 µm under the atmosphere, respectively. Moreover, the photodetectors exhibit high sensitivity in visible and near-infrared regions (8.2 mA W-1 at 650 nm and 15.6 mA W-1 at 960 nm). The power- and polarization-dependent photoresponse measurements reveal the linear relationship of power photoresponse and obvious anisotropic photoresponse (the ratio of anisotropy ellipse is 8.3 at 10.7 µm), respectively. These results suggest that the PtTe2 could be expected to be an advanced photodetection material for polarization angle-sensitive detection, infrared imaging, and photodetection from the visible to MIR range.

17.
ACS Appl Mater Interfaces ; 12(50): 56393-56402, 2020 Dec 16.
Artículo en Inglés | MEDLINE | ID: mdl-33274913

RESUMEN

Electronic materials and devices that can mimic biological systems featured with elasticity, toughness, self-healing, degradability, and environmental friendliness drive the technological developments in fields spanning from bioelectronics, biomedical diagnosis and therapy, electronic skin, and soft robotics to Internet-of-Things with "green" electronics. Among them, ionic devices based on gel electrolytes have emerged as attractive candidates for biomimetic systems. Herein, we presented a straightforward approach to demonstrate soft ionic microdevices based on a versatile organohydrogel platform acting as both a free-standing, stretchable, adhesive, healable, and entirely degradable support and a highly conductive, dehydration- and freezing-tolerant electrolyte. This is achieved by forming a gelatin/ferric-ion-cross-linked polyacrylic acid (GEL/PAA) dual dynamic supramolecular network followed by soaking into a NaCl glycerol/water solution to further toughen the gelatin network via solvent displacement, thus obtaining a high toughness of 1.34 MJ·cm-3 and a high ionic conductivity (>7 mS·cm-1). Highly stretchable and multifunctional ionic microdevices are then fabricated based on the organohydrogel electrolytes by simple transfer printing of carbon-based microelectrodes onto the prestretched gel surface. Proof-of-concept microdevices including resistive strain sensors and microsupercapacitors are demonstrated, which displayed outstanding stretchability to 300% strain, resistance to dehydration for >6 months, autonomous self-healing, and rapid room-temperature degradation within hours. The present material design and fabrication approach for the organohydrogel-based ionic microdevices will provide promising scope for life-like and sustainable electronic systems.


Asunto(s)
Electrólitos/química , Electrónica , Hidrogeles/química , Resinas Acrílicas/química , Elasticidad , Conductividad Eléctrica , Gelatina/química , Glicerol/química , Iones/química
18.
Sci Adv ; 6(39)2020 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-32967836

RESUMEN

Halide perovskites have exceptional optoelectronic properties, but a poor understanding of the relationship between crystal dimensions, composition, and properties limits their use in integrated devices. We report a new multiplexed cantilever-free scanning probe method for synthesizing compositionally diverse and size-controlled halide perovskite nanocrystals spanning square centimeter areas. Single-particle photoluminescence studies reveal multiple independent emission modes due to defect-defined band edges with relative intensities that depend on crystal size at a fixed composition. Smaller particles, but ones with dimensions that exceed the quantum confinement regime, exhibit blue-shifted emission due to reabsorption of higher-energy modes. Six different halide perovskites have been synthesized, including a layered Ruddlesden-Popper phase, and the method has been used to prepare functional solar cells based on single nanocrystals. The ability to pattern arrays of multicolor light-emitting nanocrystals opens avenues toward the development of optoelectronic devices, including optical displays.

19.
Soft Matter ; 16(38): 8736-8759, 2020 Oct 07.
Artículo en Inglés | MEDLINE | ID: mdl-32969442

RESUMEN

Surface-grafted macromolecules, including polymers, DNA, peptides, etc., are versatile modifications to tailor the interfacial functions in a wide range of fields. In this review, we aim to provide an overview of the most recent progress in engineering surface-grafted chains for the creation of complex and multiplexed surface architectures over micro- to macro-scopic areas. A brief introduction to surface grafting is given first. Then the fabrication of complex surface architectures is summarized with a focus on controlled chain conformations, grafting densities and three-dimensional structures. Furthermore, recent advances are highlighted for the generation of multiplexed arrays with designed chemical composition in both horizontal and vertical dimensions. The applications of such complicated macromolecular architectures are then briefly discussed. Finally, some perspective outlooks for future studies and challenges are suggested. We hope that this review will be helpful to those just entering this field and those in the field requiring quick access to useful reference information about the progress in the properties, processing, performance, and applications of functional surface-grafted architectures.

20.
ACS Appl Mater Interfaces ; 12(39): 44067-44073, 2020 Sep 30.
Artículo en Inglés | MEDLINE | ID: mdl-32901478

RESUMEN

The enhancement of electron-phonon interaction provides a reasonable explanation for gate-tunable phonon properties in some semiconductors where multiple inequivalent valleys are simultaneously occupied upon charge doping, especially in few-layer transition metal dichalcogenides (TMDs). In this work, we report var der Waals epitaxy of 2H-MoSe2 by molecular beam epitaxy (MBE) and gate-tunable phonon properties in monolayer and bilayer MoSe2. In monolayer MoSe2, we find that out-of-plane phonon mode A1g exhibits a strong softening and shifting toward lower wavenumbers at a high electron doping level, while in-plane phonon mode E2g1 remains unchanged. The softening and shifting of the out-of-plane phonon mode could be attributed to the increase of electron-phonon interaction and the simultaneous occupation of electrons in multiple inequivalent valleys. In bilayer MoSe2, no corresponding changes of phonon modes are detected at the same doping level, which could originate from the occupation of electrons only in single valleys upon high electron doping. This study demonstrates electrostatically enhanced electron-phonon interaction in monolayer MoSe2 and clarifies the relevance between occupation of multiple valleys and phonon properties by comparing Raman spectra of monolayer and bilayer MoSe2 at different doping levels.

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