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.
Despite broad interest in aluminum gallium nitride (AlGaN) optoelectronic devices for deep ultraviolet (DUV) applications, the performance of conventional Al(Ga)N planar devices drastically decays when approaching the AlN end, including low internal quantum efficiencies (IQEs) and high device operation voltages. Here we show that these challenges can be addressed by utilizing nitrogen (N) polar Al(Ga)N nanowires grown directly on Si substrate. By carefully tuning the synthesis conditions, a record IQE of 80% can be realized with N-polar AlN nanowires, which is nearly ten times higher compared to high quality planar AlN. The first 210 nm emitting AlN nanowire light emitting diodes (LEDs) were achieved, with a turn on voltage of about 6 V, which is significantly lower than the commonly observed 20 – 40 V. This can be ascribed to both efficient Mg doping by controlling the nanowire growth rate and N-polarity induced internal electrical field that favors hole injection. In the end, high performance N-polar AlGaN nanowire LEDs with emission wavelengths covering the UV-B/C bands were also demonstrated.
Photoelectrochemical (PEC) reduction of CO with HO not only provides an opportunity for reducing net CO emissions but also produces value-added chemical feedstocks and fuels. Syngas, a mixture of CO and H, 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 CO reduction into syngas with controlled composition owing to the difficulties associated with the chemical inertness of CO and complex reaction network of CO conversion. Herein, by employing a metal/oxide interface to spontaneously activate CO 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/H 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 CO 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 CO reduction into valuable carbon-based chemicals and fuels.
Artificial photosynthesis via solar water splitting provides a promising approach to storing solar energy in the form of hydrogen on a global scale. However, an efficient and cost-effective solar hydrogen production system that can compete with traditional methods using fossil fuels is yet to be developed. A photoelectrochemical (PEC) tandem cell consisting of a p-type photocathode and an n-type photoanode, with the photovoltage provided by the two photoelectrodes, is an attractive route to achieve highly efficient unassisted water splitting at a low cost. In this article, we provide an overview of recent developments of semiconductor materials, including metal oxides, nitrides, chalcogenides, Si, III–V compounds and organics, either as photocathodes or photoanodes for water reduction and oxidation, respectively. In addition, recent efforts in constructing a PEC tandem system for unassisted water splitting are outlined. The importance of developing a single-photon photocathode and photoanode that can deliver high photocurrent in the low bias region for efficient PEC tandem system is highlighted. Finally, we discuss the future development of photoelectrode materials, and viable solutions to realize highly efficient PEC water splitting device for practical applications.
We have investigated the quantum efficiency of monolayer MoS2 light-emitting devices through detailed temperature and power-dependent photoluminescence studies and rate equation analysis. The internal quantum efficiency can reach 45 and 8.3% at 83 and 300 K, respectively. However, efficiency droop is clearly measured with increasing carrier injection due to the unusually large Auger recombination coefficient, which is found to be ∼10(-24) cm(6)/s at room temperature, nearly 6 orders of magnitude higher than that of conventional bulk semiconductors. The significantly elevated Auger recombination in the emerging two-dimensional (2D) semiconductors is primarily an indirect process and is attributed to the abrupt bounding surfaces and the enhanced correlation, mediated by magnified Coulomb interactions, between electrons and holes confined in a 2D structure.
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