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1.
Nat Mater ; 2020 Apr 20.
Artigo em Inglês | MEDLINE | ID: mdl-32313264

RESUMO

Carrier transport processes in assemblies of nanostructures rely on morphology-dependent and hierarchical conduction mechanisms, whose complexity cannot be captured by current modelling approaches. Here we apply the concept of complex networks to modelling carrier conduction in such systems. The approach permits assignment of arbitrary connectivity and connection strength between assembly constituents and is thus ideal for nanostructured films, composites and other geometries. Modelling of simplified rod-like nanostructures is consistent with analytical solutions, whereas results for more realistic nanostructure assemblies agree with experimental data and reveal conduction behaviour not captured by previous models. Fitting of ensemble measurements also allows the conduction properties of individual constituents to be extracted, which are subsequently used to guide the realization of transparent electrodes with improved performance. A global optimization process was employed to identify geometries and properties with high potential for transparent conductors. Our intuitive discretization approach, combined with a simple solver tool, allows researchers with little computational experience to carry out realistic simulations.

2.
Nano Lett ; 2020 Mar 23.
Artigo em Inglês | MEDLINE | ID: mdl-32186886

RESUMO

We here describe a novel type of long-wavelength radiation detector that measures illumination intensity at room temperature through mechanical transduction. Compared to semiconductor-based bolometers, our nanomechanical detector exhibits low measurement noise and is inherently transparent and flexible. The presented solid-state device is based on a 2D-material film that acts as radiation absorber and detector of mechanical strain at the substrate-absorber interface. Optimization of the 2D material properties and realization of a novel edge-on device geometry combines unprecedented detectivity of 3.34 × 108 cm Hz1/2 W-1 with micrometer-scale spatial resolution. The observed combination of superior performance with the facile and scalable fabrication using only liquid processes shows the potential of the presented detector for future ubiquitous and wearable electronics.

3.
Nanoscale ; 12(7): 4751, 2020 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-32037432

RESUMO

Correction for 'Patterned liquid metal contacts for high density, stick-and-peel 2D material device arrays' by Yen-Lin Chen et al., Nanoscale, 2018, 10, 14510-14515.

4.
ACS Appl Mater Interfaces ; 11(29): 26518-26527, 2019 Jul 24.
Artigo em Inglês | MEDLINE | ID: mdl-31283174

RESUMO

Two-dimensional (2D) material nanocomposites have emerged as a material system for discovering new physical phenomena and developing novel devices. However, because of the low density of states of most two-dimensional materials such as graphene, the heterostructure of nanocomposites suffers from an enhanced depletion region, which can greatly reduce the efficiency of the charge carrier transfer and deteriorate the device performance. To circumvent this difficulty, here we propose an alternative approach by inserting a second 2D mediator with a heavy effective mass having a large density of states in-between the heterojunction of 2D nanocomposites. The mediator can effectively reduce the depletion region and form a type-II band alignment, which can speed up the dissociation of electron-hole pairs and enhance charge carrier transfer. To illustrate the principle, we demonstrate a novel stretchable photodetector based on the combination of graphene/ReS2/perovskite quantum dots. Two-dimensional ReS2 acts as a mediator in-between highly absorbing perovskite quantum dots and a high-mobility graphene channel and a thiol-based linker between the ReS2 and the perovskite. It is found that the optical sensitivity can be enhanced by 22 times. This enhancement was ascribed to the improvement of the charge transfer efficiency as evidenced by optical spectroscopy measurements. The produced photosensors are capable of reaching the highest reported value of photoresponsivity (>107 A W-1) and detectivity compared to previously studied stretchable devices. Mechanical robustness with tolerable strain up to 100% and excellent stability make our device ideal for future wearable electronics.

5.
ACS Appl Mater Interfaces ; 11(6): 6384-6388, 2019 Feb 13.
Artigo em Inglês | MEDLINE | ID: mdl-30652856

RESUMO

Lateral heterojunctions in two-dimensional (2D) materials have demonstrated potential for high-performance sensors because of the unique electrostatic conditions at the interface. The increased complexity of producing such structures, however, has prevented their widespread use. We here demonstrate the simple and scalable fabrication of heterojunctions by a one-step synthesis process that yields photodetectors with superior device performance. Catalytic conversion of a solid precursor at optimized conditions was found to produce lateral nanostructured junctions between graphene domains and 3 nm thin amorphous carbon films. Carrier transport in these heterojunctions was found to proceed by minimizing the path through the amorphous carbon barriers, which results in a self-selective Schottky emission process with high uniformity and low emission barriers. We demonstrate the potential of thus produced heterojunctions by realizing a photodetector that combines an ultrahigh detectivity of 1013 Jones with microsecond response time, which represents the highest performance of 2D material heterojunction devices. These attractive features are retained even for millimeter-scale devices, and the demonstrated ability to produce transparent, patterned, and flexible sensors extends lateral heterojunction sensors toward wearable and large-scale electronics.

6.
ACS Appl Mater Interfaces ; 11(4): 4649-4653, 2019 Jan 30.
Artigo em Inglês | MEDLINE | ID: mdl-30628434

RESUMO

Light-based information processing has the potential to increase speed, security, and scalability of electronic devices if issues in the device complexity could be resolved. We here demonstrate an integrated nanoelectronic device that can combine, store, and manipulate optical and electronic information. Employing a mechanically flexible and multilayered structure, a device is realized that shows memristive behavior. Illumination is shown to control the device operation in several unique ways. First, the device produces photocurrent that allows us to read out the device state in a self-powered manner. More importantly, a varying light intensity modulates the switching transition in a proportional manner that is akin to a neuron with variable plasticity and which can be taught and queried using either light or electrical inputs. This behavior enables a multilevel light-controlled logic and teaching schemes that can be applied to light-based communication devices and provides a route toward ubiquitous and low-cost sensors for future internet of things applications.

7.
Sci Rep ; 9(1): 257, 2019 Jan 22.
Artigo em Inglês | MEDLINE | ID: mdl-30670729

RESUMO

The quality of CVD-grown graphene is limited by the parallel nucleation of grains from surface impurities which leads to increased grain boundary densities. Currently employed cleaning methods cannot completely remove surface impurities since impurity diffusion from the bulk to the surface occurs during growth. We here introduce a new method to remove impurities not only on the surface but also from the bulk. By employing a solid cap during annealing that acts as a sink for impurities and leads to an enhancement of copper purity throughout the catalyst thickness. The high efficiency of the solid-diffusion-based transport pathway results in a drastic decrease in the surface particle concentration in a relatively short time, as evident in AFM and SIMS characterization of copper foils. Graphene grown on those substrates displays enhanced grain sizes and room-temperature, large-area carrier mobilities in excess of 5000 cm2/Vs which emphasizes the suitability of our approach for future graphene applications.

8.
Nanoscale ; 11(3): 1074-1079, 2019 Jan 17.
Artigo em Inglês | MEDLINE | ID: mdl-30574652

RESUMO

Carrier transport in a wide range of nanomaterial assemblies proceeds by percolation through discontinuous networks of constituents. Improving percolative nanomaterials could enhance transparent conductors, sensors, and electronic devices. A significant obstacle in optimizing percolative materials is the challenge in their characterization. The critical connection pathways which determine a percolative material's conductivity are not easily accessible with existing metrology tools and traditional investigation approaches rely on indirect methods based on many samples and on simplifying assumptions. We here demonstrate the direct extraction of characteristic parameters from a single sample by analyzing the strain-dependent resistance of percolative materials. An analytical model is derived that can explain experimental data for various percolative materials, morphologies, and straining conditions. The relationship of the extracted parameters with previously introduced figures of merit allows us to compare nanostructures of diverse dimensionalities and compositions for applications such as strain gauges and transparent conductors.

9.
Nanoscale ; 10(30): 14510-14515, 2018 Aug 02.
Artigo em Inglês | MEDLINE | ID: mdl-30024009

RESUMO

Two-dimensional materials have shown great promise to enable novel wearable electronic devices ranging from sensors to energy generators. These developments are due to their high mechanical robustness, which allow them to retain high performance even at large deformations. Under these conditions, however, good electrical contacts become an important issue that cannot be addressed with conventional materials. Liquid metals could overcome this limitation by providing soft and compliant electrodes but to date no realistic heterointegration of nanomaterials and complex liquid metal contacts has been attempted. We here demonstrate the application of micrometer-sized electrical contacts to flexible, fragile and rough 2D materials using patterned liquid metal contacts. A novel deposition method enables the scalable and facile production of large arrays of contacts in arbitrary geometries. This ability permitted the single-step, fabrication-free and contamination-free production of concentric liquid metal-contacted graphene field effect transistors of comparable performance to traditional devices. We demonstrate that the contacts can be removed without damaging the 2D materials allowing the contacts to be reused. Finally, good contact could be made to complex morphologies and three-dimensional substrates, which highlights the potential of our approach to the characterization and application of nanomaterials in electronics.

10.
Sci Rep ; 8(1): 4046, 2018 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-29511308

RESUMO

Chemical vapor deposition (CVD) is promising for the large scale production of graphene and other two-dimensional materials. Optimization of the CVD process for enhancing their quality is a focus of ongoing effort and significant progress has been made in decreasing the defectiveness associated with grain boundaries and nucleation spots. However, little is known about the quality and origin of structural defects in the outgrowing lattice which are present even in single-crystalline material and represent the limit of current optimization efforts. We here investigate the formation kinetics of such defects by controlling graphene's growth rate over a wide range using nanoscale confinements. Statistical analysis of Raman spectroscopic results shows a clear trend between growth rate and defectiveness that is in quantitative agreement with a model where defects are healed preferentially at the growth front. Our results suggest that low growth rates are required to avoid the freezing of lattice defects and form high quality material. This conclusion is confirmed by a fourfold enhancement in graphene's carrier mobility upon optimization of the growth rate.

12.
Sci Rep ; 7(1): 9052, 2017 08 22.
Artigo em Inglês | MEDLINE | ID: mdl-28831126

RESUMO

Graphene's attractiveness in many applications is limited by its high resistance. Extrinsic doping has shown promise to overcome this challenge but graphene's performance remains below industry requirements. This issue is caused by a limited charge transfer efficiency (CTE) between dopant and graphene. Using AuCl3 as a model system, we measure CTE as low as 5% of the expected values due to the geometrical capacitance of small adsorbate clusters. We here demonstrate a strategy for enhancing the CTE by a two-step optimization of graphene's surface energy prior to AuCl3 doping. First, exposure to UV ozone modified the hydrophilicity of graphene and was found to decrease the cluster's geometric capacitance, which had a direct effect on the CTE. Occurrence of lattice defects at high UV exposure, however, deteriorated graphene's transport characteristics and limited the effectiveness of this pretreatment step. Thus, prior to UV exposure, a functionalized polymer layer was introduced that could further enhance graphene's surface energy while protecting it from damage. Combination of these treatment steps were found to increase the AuCl3 charge transfer efficiency to 70% and lower the sheet resistance to 106 Ω/γ at 97% transmittance which represents the highest reported performance for doped single layer graphene and is on par with commercially available transparent conductors.

13.
ACS Appl Mater Interfaces ; 9(27): 22911-22917, 2017 Jul 12.
Artigo em Inglês | MEDLINE | ID: mdl-28597658

RESUMO

Corrosion protection of complex surface is an active area of research due to its importance to commercial applications such as electrochemical fabrication. However, conventional coatings exhibit limited conductivity, thermal stability, and durability and are thus not suitable. Recent work has shown the potential of graphene, a two-dimensional carbon allotrope, for corrosion protection. The studies, however, limited themselves to simple planar geometries that provide limited insight in the applicability to relevant morphologies such as mesh electrodes and roughened surfaces. We here study the corrosion protection ability of tubular graphene (TG) on Ni-wires as a model system for such complex geometries. TG-covered Ni wires of approximately 50 µm diameters were produced by the annealing of cellulose acetate (CA) on Ni. The high quality of the TG coating was confirmed by Raman spectroscopy, scanning electron microscopy, and electrical measurements. We show that the graphene layer number could be controlled by adjusting the CA membrane quantity. We found a direct relation between the degree of corrosion inhibition with the variation of graphene layer number. The increase of graphene layers on a Ni surface could enhance its corrosion inhibition in acidic, basic, and marine environments, which shows the potential of our approach for future applications.

14.
Adv Mater ; 29(3)2017 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-27869343

RESUMO

The integration of a light-emitting transistor based on graphene/insulator/semiconductor with downconversion emitters enables the manipulation of emitted light covering the whole chromaticity space, including white-light emission. This novel arbitrary-color light emitter offers a promising approach for new applications in optoelectronic devices ranging from displays to solid-state lighting.

15.
Sci Rep ; 6: 31475, 2016 08 10.
Artigo em Inglês | MEDLINE | ID: mdl-27507171

RESUMO

The advent of 2D materials integration has enabled novel heterojunctions where carrier transport proceeds thrsough different ultrathin layers. We here demonstrate the potential of such heterojunctions on a graphene/dielectric/semiconductor vertical stack that combines several enabling features for optoelectronic devices. Efficient and stable light emission was achieved through carrier tunneling from the graphene injector into prominent states of a luminescent material. Graphene's unique properties enable fine control of the band alignment in the heterojunction. This advantage was used to produce vertical tunneling-injection light-emitting transistors (VtiLET) where gating allows adjustment of the light emission intensity independent of applied bias. This device was shown to simultaneously act as a light detecting transistor with a linear and gate tunable sensitivity. The presented development of an electronically controllable multifunctional light emitter, light detector and transistor open up a new route for future optoelectronics.

16.
Nanotechnology ; 27(10): 105602, 2016 Mar 11.
Artigo em Inglês | MEDLINE | ID: mdl-26861850

RESUMO

The production of large-scale, single crystalline graphene is a requirement for enhancing its electronic, mechanical, and chemical properties. Chemical vapor deposition (CVD) has shown the potential to grow high quality graphene but the simultaneous nucleation of many grains limits their achievable domain size. We report here that ultralow nucleation densities can be achieved through multi-step optimization of the catalyst morphology. First, annealing in a hydrogen-free environment is required to retain a surface copper oxide which decreases the nucleation density. Second, CuO was found to be the relevant copper species for this process and air oxidation of the copper foil at 200 °C maximizes its concentration. Both pre-treatment steps were found to affect the morphology of the catalyst and a direct correlation between nucleation density and surface roughness was found which indicates that the primary role of the oxidation step is the decrease in catalyst roughness. To further enhance this determining parameter, confined CVD was carried out after sample oxidation and hydrogen-free annealing. Each of these three steps reduces the grain density by approximately one order of magnitude resulting in ultralow nucleation densities of 1.23 grains/mm(2) and high quality, single-crystalline graphene grains of several millimeter sizes were grown using this method.

17.
Nanoscale ; 8(3): 1327-31, 2016 Jan 21.
Artigo em Inglês | MEDLINE | ID: mdl-26689362

RESUMO

A high carrier mobility is an important parameter for graphene-based electronics. While the recent reports have shown impressive results for individual micro-scale devices, scalable production of high mobility graphene has been challenging. We here show that centimeter-scale graphene devices with room temperature carrier mobilities in excess of 10 000 cm(2) V(-1) s(-1) can be achieved on polyolefinic substrates. Measurements on Parafilm-supported graphene devices show, on average, a fivefold-enhancement in mobility over traditional devices. We find that a decreased charged-impurity scattering is the origin of this behavior. Spectroscopic characterization reveals oxygen-containing polymer residue as the main source of such charged impurities. A comparison of different polyolefins highlights the positive impact of oxygen-free polymers as support materials for high mobility graphene devices. Finally, moldable and wearable graphene devices for biosensors were shown to be enabled by polyolefinic substrates.

18.
Phys Chem Chem Phys ; 18(1): 339-43, 2016 Jan 07.
Artigo em Inglês | MEDLINE | ID: mdl-26617396

RESUMO

Graphene's unique semimetallic band structure yields carriers with widely tunable energy levels that enable novel electronic devices and energy generators. To enhance the potential of this feature, a scalable synthesis method for graphene with adjustable Fermi levels is required. We here show that the electrochemical intercalation of FeCl3 and subsequent electrochemical exfoliation produces graphene whose energy levels can be finely tuned by the intercalation parameters. X-ray photoelectron spectroscopy reveals that a gradual transition in the bonding character of the intercalant is the source of this behavior. The intercalated graphene exhibits a significantly increased work function that can be varied between 4.8 eV and 5.2 eV by the intercalation potential. Transparent conducting electrodes produced by these graphene flakes exhibit a threefold improvement in performance and the doping effect was found to be stable for more than a year. These findings open up a new route for the scalable production of graphene with adjustable properties for future applications.

19.
Sci Rep ; 5: 17393, 2015 Nov 30.
Artigo em Inglês | MEDLINE | ID: mdl-26617255

RESUMO

Graphene's low intrinsic carrier concentration necessitates extrinsic doping to enhance its conductivity and improve its performance for application as electrodes or transparent conductors. Despite this importance limited knowledge of the doping process at application-relevant conditions exists. Employing in-situ carrier transport and Raman characterization of different dopants, we here explore the fundamental mechanisms limiting the effectiveness of doping at different doping levels. Three distinct transport regimes for increasing dopant concentration could be identified. First the agglomeration of dopants into clusters provides a route to increase the graphene conductivity through formation of ordered scatterers. As the cluster grows, the charge transfer efficiency between graphene and additional dopants decreases due to emerging polarization effects. Finally, large dopant clusters hinder the carrier motion and cause percolative transport that leads to an unexpected change of the Hall effect. The presented results help identifying the range of beneficial doping density and guide the choice of suitable dopants for graphene's future applications.

20.
Nanoscale ; 7(46): 19403-7, 2015 Dec 14.
Artigo em Inglês | MEDLINE | ID: mdl-26537536

RESUMO

Graphene's impact on future applications is intimately linked to advances in the synthesis of high quality materials. Chemical vapor deposition (CVD) shows great potential in this area but insufficient connectivity between single-crystalline domains deteriorates the achievable electrical and mechanical performance. We here demonstrate that the inter-grain connectivity can be significantly improved by adding a second material in the vicinity of the growth substrate. This promoter decreases the amount of structural defects that remain at the grain boundaries of conventionally grown graphene even after 6 hour growth. A two-step growth process was employed to selectively enhance the grain connectivity while maintaining an identical graphene grain morphology with and without a promoter. Graphite was found to yield the largest enhancement in the connectivity of graphene grains due to its high catalytic activity compared to other promoter materials. A novel cap-design ensured a large scale and uniform improvement of the inter-grain connectivity results which led to an enhancement of large scale carrier mobilities from 2700 cm(2) V(-1) s(-1) to 4000 cm(2) V(-1) s(-1) and highlights the potential of our approach to improving the connectivity of CVD-grown graphene.

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