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1.
Nat Commun ; 9(1): 3856, 2018 09 21.
Artigo em Inglês | MEDLINE | ID: mdl-30242212

RESUMO

The combination of earth-abundant catalysts and semiconductors, for example, molybdenum sulfides and planar silicon, presents a promising avenue for the large-scale conversion of solar energy to hydrogen. The inferior interface between molybdenum sulfides and planar silicon, however, severely suppresses charge carrier extraction, thus limiting the performance. Here, we demonstrate that defect-free gallium nitride nanowire is ideally used as a linker of planar silicon and molybdenum sulfides to produce a high-quality shell-core heterostructure. Theoretical calculations revealed that the unique electronic interaction and the excellent geometric-matching structure between gallium nitride and molybdenum sulfides enabled an ideal electron-migration channel for high charge carrier extraction efficiency, leading to outstanding performance. A benchmarking current density of 40 ± 1 mA cm-2 at 0 V vs. reversible hydrogen electrode, the highest value ever reported for a planar silicon electrode without noble metals, and a large onset potential of +0.4 V were achieved under standard one-sun illumination.

2.
J Am Chem Soc ; 140(25): 7869-7877, 2018 06 27.
Artigo em Inglês | MEDLINE | ID: mdl-29905471

RESUMO

Photoelectrochemical (PEC) reduction of CO2 with H2O not only provides an opportunity for reducing net CO2 emissions but also produces value-added chemical feedstocks and fuels. Syngas, a mixture of CO and H2, is a key feedstock for the production of methanol and other commodity hydrocarbons in industry. However, it is challenging to achieve efficient and stable PEC CO2 reduction into syngas with controlled composition owing to the difficulties associated with the chemical inertness of CO2 and complex reaction network of CO2 conversion. Herein, by employing a metal/oxide interface to spontaneously activate CO2 molecule and stabilize the key reaction intermediates, we report a benchmarking solar-to-syngas efficiency of 0.87% and a high turnover number of 24 800, as well as a desirable high stability of 10 h. Moreover, the CO/H2 ratios in the composition can be tuned in a wide range between 4:1 and 1:6 with a total unity Faradaic efficiency. On the basis of experimental measurements and theoretical calculations, we present that the metal/oxide interface provides multifunctional catalytic sites with complementary chemical properties for CO2 activation and conversion, leading to a unique pathway that is inaccessible with the individual components. The present approach opens new opportunities to rationally develop high-performance PEC systems for selective CO2 reduction into valuable carbon-based chemicals and fuels.

3.
Nanoscale Res Lett ; 12(1): 488, 2017 Aug 10.
Artigo em Inglês | MEDLINE | ID: mdl-28799071

RESUMO

We demonstrate that the atom chain structure of Te allows it to be exfoliated as ultra-thin flakes and nanowires. Atomic force microscopy of exfoliated Te shows that thicknesses of 1-2 nm and widths below 100 nm can be exfoliated with this method. The Raman modes of exfoliated Te match those of bulk Te, with a slight shift (4 cm-1) due to a hardening of the A1 and E modes. Polarized Raman spectroscopy is used to determine the crystal orientation of exfoliated Te flakes. These experiments establish exfoliation as a route to achieve nanoscale trigonal Te while also demonstrating the potential for fabrication of single atom chains of Te.

4.
Nano Lett ; 15(8): 5302-6, 2015 Aug 12.
Artigo em Inglês | MEDLINE | ID: mdl-26214363

RESUMO

The discovery of direct bandgap semiconducting two-dimensional (2D) transition metal dichalcogenides (TMDCs) has opened a new era in flexible optoelectronic devices. Critical to this development is the realization of a semiconductor laser using the emerging 2D TMDCs. Here, by embedding 2D MoS2 at the interface between a free-standing microdisk and microsphere, we have demonstrated, for the first time, room-temperature lasing from 2D TMDCs. The devices exhibit multiple lasing peaks in the wavelength range of ∼600 to 800 nm. The threshold is measured to be ∼5 µW under continuous wave operation at room temperature. No saturation in the output power is measured for pump powers more than 2 orders of magnitude larger than the threshold. The superior performance is attributed to the large gain of 2D TMDCs and the strong coupling between the 2D MoS2 gain medium and optical modes in the unique optical cavity.

5.
Sci Rep ; 5: 7744, 2015 Jan 16.
Artigo em Inglês | MEDLINE | ID: mdl-25592057

RESUMO

We report on the demonstration of a new type of axial nanowire LED heterostructures, with the use of self-organized InGaN/AlGaN dot-in-a-wire core-shell nanowire arrays. The large bandgap AlGaN shell is spontaneously formed on the sidewall of the nanowire during the growth of AlGaN barrier of the quantum dot active region. As such, nonradiative surface recombination, that dominates the carrier dynamics of conventional axial nanowire LED structures, can be largely eliminated, leading to significantly increased carrier lifetime from ~0.3 ns to 4.5 ns. The luminescence emission is also enhanced by orders of magnitude. Moreover, the p-doped AlGaN barrier layers can function as distributed electron blocking layers (EBLs), which is found to be more effective in reducing electron overflow, compared to the conventional AlGaN EBL. The device displays strong white-light emission, with a color rendering index of ~95. An output power of >5 mW is measured for a 1 mm × 1 mm device, which is more than 500 times stronger than the conventional InGaN axial nanowire LEDs without AlGaN distributed EBLs.

6.
Opt Express ; 22 Suppl 7: A1768-75, 2014 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-25607491

RESUMO

We demonstrate controllable and tunable full color light generation through the monolithic integration of blue, green/yellow, and orange/red InGaN nanowire light-emitting diodes (LEDs). Such multi-color nanowire LED arrays are fabricated directly on Si substrate using a three-step selective area molecular beam epitaxy growth process. The lateral-arranged multi-color subpixels enable controlled light mixing at the chip-level and yield color-tunable light emission with CCT values in the range from 1900 K to 6800 K, while maintaining excellent color rendering capability. This work provides a viable approach for achieving micron and nanoscale tunable full-color LED arrays without the compromise between the device efficiency and light quality associated with conventional phosphor-based LEDs.

7.
Nano Lett ; 13(11): 5437-42, 2013.
Artigo em Inglês | MEDLINE | ID: mdl-24074440

RESUMO

We have examined the carrier injection process of axial nanowire light-emitting diode (LED) structures and identified that poor carrier injection efficiency, due to the large surface recombination, is the primary cause for the extremely low output power of phosphor-free nanowire white LEDs. We have further developed InGaN/GaN/AlGaN dot-in-a-wire core-shell white LEDs on Si substrate, which can break the carrier injection efficiency bottleneck, leading to a massive enhancement in the output power. At room temperature, the devices can exhibit an output power of ~1.5 mW, which is more than 2 orders of magnitude stronger than nanowire LEDs without shell coverage. Additionally, such phosphor-free nanowire white LEDs can deliver an unprecedentedly high color rendering index of ~92-98 in both the warm and cool white regions, with the color rendering capability approaching that of an ideal light source, i.e. a blackbody.

8.
Nanotechnology ; 21(13): 134020, 2010 Apr 02.
Artigo em Inglês | MEDLINE | ID: mdl-20208120

RESUMO

Top emission organic light emitting diodes (OLEDs) with carbon nanotubes (CNTs) as top electrodes were fabricated and characterized. Devices were fabricated on glass substrates with evaporated bottom Al/LiF cathodes, a spin coated organic emissive layer and a PEDOT-PSS hole injection layer. Transparent thin CNT films were deposited on top of the emission layer to form the anode by micro-contact printing with a polydimethylsiloxane stamp. A very good device performance was obtained, with a peak luminance of 3588 cd m(-2) and a maximum current efficiency of 1.24 cd A(-1). This work shows the possibility of using CNTs as transparent electrodes to replace ITO in organic semiconductor devices. Furthermore, the top emission nature of such devices offers a broader range of applications of CNTs on any type of substrate. By combining with solution processed organic materials, it is anticipated that lower cost fabrication will be possible through roll-to-roll manufacture.

9.
Nanotechnology ; 21(12): 125201, 2010 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-20182012

RESUMO

We report on the achievement of planar memristive devices on monocrystalline ZnO substrates using Ti/Al and Pt/Au contacts with dimensions of 100 x 100 microm(2) and spacings of approximately 60 microm. Effects of both thermal and electro-forming processes on the switching characteristics are investigated. It is observed that the thermally formed devices exhibit an extremely large R(OFF)/R(ON) value of approximately 20 000. The electrically formed devices, on the other hand, demonstrate an exceptional switching stability, with R(OFF)/R(ON) variations of < 2% for durations of over 10(5) s and more than 1800 switching cycles. The dependence of the switching characteristics on the formation processes, as well as the metal electrodes, could be explained by an oxygen vacancy formation/annihilation and migration model.

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