Two-dimensional semiconductors such as MoS2 are an emerging material family with wide-ranging potential applications in electronics, optoelectronics, and energy harvesting. Large-area growth methods are needed to open the way to applications. Control over lattice orientation during growth remains a challenge. This is needed to minimize or even avoid the formation of grain boundaries, detrimental to electrical, optical, and mechanical properties of MoS2 and other 2D semiconductors. Here, we report on the growth of high-quality monolayer MoS2 with control over lattice orientation. We show that the monolayer film is composed of coalescing single islands with limited numbers of lattice orientation due to an epitaxial growth mechanism. Optical absorbance spectra acquired over large areas show significant absorbance in the high-energy part of the spectrum, indicating that MoS2 could also be interesting for harvesting this region of the solar spectrum and fabrication of UV-sensitive photodetectors. Even though the interaction between the growth substrate and MoS2 is strong enough to induce lattice alignment via van der Waals interaction, we can easily transfer the grown material and fabricate devices. Local potential mapping along channels in field-effect transistors shows that the single-crystal MoS2 grains in our film are well connected, with interfaces that do not degrade the electrical conductivity. This is also confirmed by the relatively large and length-independent mobility in devices with a channel length reaching 80 μm.
Light management is of great importance in photovoltaic cells, as it determines the fraction of incident light entering the device. An optimal p-n junction combined with optimal light absorption can lead to a solar cell efficiency above the Shockley-Queisser limit. Here, we show how this is possible by studying photocurrent generation for a single core-shell p-i-n junction GaAs nanowire solar cell grown on a silicon substrate. At 1 sun illumination, a short-circuit current of 180 mA cm -2 is obtained, which is more than one order of magnitude higher than that predicted from the Lambert-Beer law. The enhanced light absorption is shown to be due to a light-concentrating property of the standing nanowire, as shown by photocurrent maps of the device. The results imply new limits for the maximum efficiency obtainable with III-V based nanowire solar cells under 1 sun illumination.N anowire-based solar cells hold great promise for third-generation photovoltaics and for powering nanoscale devices 1,2 . With the advent of third-generation photovoltaics, solar cells will become cheaper and more efficient than current devices. In particular, a cost reduction may be achieved by reducing material use through the fabrication of nanowire arrays and radial p-n junctions [3][4][5] . The geometry of nanowire crystals is expected to favour elastic strain relaxation, providing great freedom in the design of new compositional multijunction solar cells 6 grown on mismatched materials 7,8 . The efficiencies of nanostructured solar cells have increased over time and have now reached up to 13.8%, due to improvements in materials and new device concepts [9][10][11][12][13][14] .Light absorption in standing nanowires is a complex phenomenon, with a strong dependence on nanowire dimensions and the absorption coefficient of the raw materials [15][16][17][18] . In low-absorbing microwire arrays, such as those composed of silicon, light absorption is understood via ray optics or by calculation of the integrated local density of optical states of the nanowire film 19,20 . Interestingly, when these arrays stand on a Lambertian back-reflector, an asymptotic increase in light trapping for low filling factors (FFs) is predicted 19 . This is advantageous for improvement of the efficiency-to-cost ratio of solar cells and has led to the demonstration of microwire arrays exhibiting higher absorption than in the equivalent thickness of textured film 19,21,22 . The case for nanowires is quite different. Nanowire diameters are smaller than or comparable to the radiation wavelength. In this case, optical interference and guiding effects play a dominant role in relation to reflectivity and absorption spectra. For low-absorbing materials (for example, indirect bandgap materials such as silicon), waveguiding effects plays a key role 23,24 , whereas highly absorbing semiconductors (such as direct-bandgap GaAs) exhibit resonances that increase the total absorption several times. Nanowires lying on a substrate also exhibit such resonances, often described by Mi...
The structural and optical properties of three different kinds of GaAs nanowires with 100% zinc-blende structure and with an average of 30% and 70% wurtzite are presented. A variety of shorter and longer segments of zinc-blende or wurtzite crystal phases are observed by transmission electron microscopy in the nanowires. Sharp photoluminescence lines are observed with emission energies tuned from 1.515 eV down to 1.43 eV when the percentage of wurtzite is increased. The downward shift of the emission peaks can be understood by carrier confinement at the interfaces, in quantum wells and in random short period superlattices existent in these nanowires, assuming a staggered band offset between wurtzite and zinc-blende GaAs. The latter is confirmed also by time-resolved measurements. The extremely local nature of these optical transitions is evidenced also by cathodoluminescence measurements. Raman spectroscopy on single wires shows different strain conditions, depending on the wurtzite content which affects also the band alignments. Finally, the occurrence of the two crystallographic phases is discussed in thermodynamic terms.
Quantum dots embedded within nanowires represent one of the most promising technologies for applications in quantum photonics. Whereas the top-down fabrication of such structures remains a technological challenge, their bottom-up fabrication through self-assembly is a potentially more powerful strategy. However, present approaches often yield quantum dots with large optical linewidths, making reproducibility of their physical properties difficult. We present a versatile quantum-dot-innanowire system that reproducibly self-assembles in core-shell GaAs/AlGaAs nanowires. The quantum dots form at the apex of a GaAs/AlGaAs interface, are highly stable, and can be positioned with nanometre precision relative to the nanowire centre. Unusually, their emission is blue-shifted relative to the lowest energy continuum states of the GaAs core. Large-scale electronic structure calculations show that the origin of the optical transitions lies in quantum confinement due to Al-rich barriers. By emitting in the red and self-assembling on silicon substrates, these quantum dots could therefore become building blocks for solid-state lighting devices and third-generation solar cells. S emiconductor quantum dots have been shown to be excellent building blocks for quantum photonics applications, such as single-photon sources and nano-sensing. Desirable properties of a single-photon emitter include high-fidelity anti-bunching (very small g 2 (t = 0)), narrow emission lines (ideally transform limited to a few microelectronvolt) and high brightness (>1 MHz count rate on standard detector). For simplicity, these properties should be achieved either with electrical injection or non-resonant optical excitation. Desirable properties of a nano-sensor include a high sensitivity to local electric and magnetic fields, with the quantum dot located as close as possible to the target region. A popular realization involves Stranski-Krastanow InGaAs quantum dots embedded in a three-dimensional matrix, which are excellent building blocks for the realization of practical singlephoton sources 1 . However, the photon extraction out of the bulk semiconductor is highly inefficient on account of the large mismatch in refractive indices of GaAs and vacuum. An attractive way forward is to embed the quantum dots in a nanowire 2 . To solve the extraction problem, the nanowire is designed to operate as a single-mode waveguide, a so-called photonic nanowire, with a taper as photon out-coupler 3 . Also, for nano-sensing applications, a quantum dot in a nanowire can be located much closer to the active medium. Top-down fabrication of the photonic waveguide is technologically complex, however. Bottom-up fabrication of the photonic waveguide is very attractive 4-6 , but it is at present challenging to self-assemble quantum dots in the nanowires with narrow linewidths and high yields 7,8 . Nano-sensing applications are at present not highly developed. Other degrees of freedom of the quantum-dot-in-nanowire system that can be usefully exploited are the mechanical modes ...
Two-dimensional (2D) materials are a new type of materials under intense study because of their interesting physical properties and wide range of potential applications from nanoelectronics to sensing and photonics. Monolayers of semiconducting transition metal dichalcogenides MoS2 or WSe2 have been proposed as promising channel materials for field-effect transistors. Their high mechanical flexibility, stability, and quality coupled with potentially inexpensive production methods offer potential advantages compared to organic and crystalline bulk semiconductors. Due to quantum mechanical confinement, the band gap in monolayer MoS2 is direct in nature, leading to a strong interaction with light that can be exploited for building phototransistors and ultrasensitive photodetectors. Here, we report on the realization of light-emitting diodes based on vertical heterojunctions composed of n-type monolayer MoS2 and p-type silicon. Careful interface engineering allows us to realize diodes showing rectification and light emission from the entire surface of the heterojunction. Electroluminescence spectra show clear signs of direct excitons related to the optical transitions between the conduction and valence bands. Our p–n diodes can also operate as solar cells, with typical external quantum efficiency exceeding 4%. Our work opens up the way to more sophisticated optoelectronic devices such as lasers and heterostructure solar cells based on hybrids of 2D semiconductors and silicon.
Molecular beam epitaxy Ga-assisted synthesis of GaAs nanowires is demonstrated. The nucleation and growth are seen to be related to the presence of a SiO 2 layer previously deposited on the GaAs wafer. The interaction of the reactive gallium with the SiO 2 pinholes induces the formation of nanocraters, found to be the key for the nucleation of the nanowires. With SiO 2 thicknesses up to 30 nm, nanocraters reach the underlying substrate, resulting into a preferential growth orientation of the nanowires. Possibly related to the formation of nanocraters, we observe an incubation period of 258 s before the nanowires growth is initiated. © 2008 American Institute of Physics. ͓DOI: 10.1063/1.2837191͔Semiconductor nanowires are believed to play a decisive role in the electronic and optoelectronic devices of the 21st century. Up to now, the synthesis of nanowires is mainly based on the vapor-liquid-solid and vapor-solid-solid mechanisms. 1,2 Common in both mechanisms is that a metal nanoparticle gathers and decomposes catalytically the precursor molecules. Supersaturation of the metal droplet follows and leads to the precipitation of a solid phase underneath the droplet in the form of a nanowire. Typically, gold is used as a catalyst. The use of such an extrinsic catalytic metal is in general not desired and some effort has been directed into finding alternatives. 3,4 Recently, catalyst-free growth has been achieved both with metal-organic chemical vapor deposition and molecular beam epitaxy ͑MBE͒. 5,6 This type of growth has always been linked to the existence of a plain or patterned SiO 2 surface, whose role has still to be clarified. To our knowledge, a detailed study on the nucleation stage of the nanowires and an analysis of the role of the SiO 2 are still missing.Nanowires were grown in a Gen-II MBE system. 2 in. GaAs wafers were sputtered with silicon dioxide; the thickness was varied between 20 and 100 nm. In order to ensure a contamination-free surface, the substrates were dipped for 2 s in a 12% HF aqueous solution, nitrogen blow dried, and were immediately after transferred in the load lock of the growth chamber. In order to desorb any remnant adsorbed molecules at the surface, the wafers were heated to 650°C for 30 min prior to growth. The synthesis was carried out at a temperature of 630°C, an arsenic As 4 partial pressure of 8 ϫ 10 −7 mbar, a Ga rate of 0.25 Å / s and under rotation of 4 rpm.We first discuss nanowires which were grown simultaneously on two different halves of GaAs substrates with the ͑001͒ and ͑111͒B orientations. After cleaning of the surface and HF dip, the two halves were still coated with a 6 nm SiO 2 thin film. Cross-sectional scanning electron microscopy ͑SEM͒ measurements of the grown nanowires are shown in Fig. 1. The micrographs clearly reveal that the nanowires mainly grow perpendicular to the substrate in the case of the ͑111͒B GaAs, and with an angle of ϳ35°in the case of the ͑001͒ GaAs. This result clearly proves the existence of a relation between the nanowire orientation and...
Polarization-dependent Raman scattering experiments realized on single GaAs nanowires with different percentages of zinc-blende and wurtzite structure are presented. The selection rules for the special case of nanowires are found and discussed. In the case of zinc-blende, the transversal optical mode E 1 ͑TO͒ at 267 cm −1 exhibits the highest intensity when the incident and analyzed polarization are parallel to the nanowire axis. This is a consequence of the nanowire geometry and dielectric mismatch with the environment, and in quite good agreement with the Raman selection rules. We also find a consistent splitting of 1 cm −1 of the E 1 ͑TO͒. The transversal optical mode related to the wurtzite structure, E 2 H , is measured between 254 and 256 cm −1 , depending on the wurtzite content. The azimuthal dependence of E 2 H indicates that the mode is excited with the highest efficiency when the incident and analyzed polarization are perpendicular to the nanowire axis, in agreement with the selection rules. The presence of strain between wurtzite and zinc-blende is analyzed by the relative shift of the E 1 ͑TO͒ and E 2 H modes. Finally, the influence of the surface roughness in the intensity of the longitudinal optical mode on ͕110͖ facets is presented.
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