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 ...
We experimentally demonstrate the directional emission of polarized light from single semiconductor nanowires. The directionality of this emission has been directly determined with Fourier microphotoluminescence measurements of vertically oriented InP nanowires. Nanowires behave as efficient optical nanoantennas, with emission characteristics that are not only given by the material but also by their geometry and dimensions. By means of finite element simulations, we show that the radiated power can be enhanced for frequencies and diameters at which leaky modes in the structure are present. These leaky modes can be associated to Mie resonances in the cylindrical structure. The radiated power can be also inhibited at other frequencies or when the coupling of the emission to the resonances is not favored. We anticipate the relevance of these results for the development of nanowire photon sources with optimized efficiency and/or controlled emission by the geometry.
We show that optically active quantum dots (QDs) embedded in MBE-grown GaAs/AlGaAs core-shell nanowires (NWs) are coupled to the NW mechanical motion. Oscillations of the NW modulate the QD emission energy in a broad range exceeding 14 meV. Furthermore, this opto-mechanical interaction enables the dynamical tuning of two neighboring QDs into resonance, possibly allowing for emitter-emitter coupling. Both the QDs and the coupling mechanism, i.e. material strain, are intrinsic to the NW structure and do not depend on any functionalization or external field. Such systems open up the prospect of using QDs to probe and control the mechanical state of a NW, or conversely of making a quantum nondemolition readout of a QD state through a position measurement.
Carbon nanostructures that feature two-dimensional extended nanosheets are important components for technological applications such as high-performance composites, lithium-ion storage, photovoltaics and nanoelectronics. Chemical functionalization would render such structures better processable and more suited for tailored applications, but typically this is precluded by the high temperatures needed to prepare the nanosheets. Here, we report direct access to functional carbon nanosheets of uniform thickness at room temperature. We used amphiphiles that contain hexayne segments as metastable carbon precursors and self-assembled these into ordered monolayers at the air/water interface. Subsequent carbonization by ultraviolet irradiation in ambient conditions resulted in the quantitative carbonization of the hexayne sublayer. Carbon nanosheets prepared in this way retained their surface functionalization and featured an sp(2)-rich amorphous carbon structure comparable to that usually obtained on annealing above 800 °C. Moreover, they exhibited a molecularly defined thickness of 1.9 nm, were mechanically self-supporting over several micrometres and had macroscopic lateral dimensions on the order of centimetres.
Nanowire diameter has a dramatic effect on the absorption cross-section in the optical domain. The maximum absorption is reached for ideal nanowire morphology within a solar cell device. As a consequence, understanding how to tailor the nanowire diameter and density is extremely important for high-efficient nanowire-based solar cells. In this work, we investigate mastering the diameter and density of self-catalyzed GaAs nanowires on Si(111) substrates by growth conditions using the self-assembly of Ga droplets. We introduce a new paradigm of the characteristic nucleation time controlled by group III flux and temperature that determine diameter and length distributions of GaAs nanowires. This insight into the growth mechanism is then used to grow nanowire forests with a completely tailored diameter-density distribution. We also show how the reflectivity of nanowire arrays can be minimized in this way. In general, this work opens new possibilities for the cost-effective and controlled fabrication of the ensembles of self-catalyzed III-V nanowires for different applications, in particular in next-generation photovoltaic devices.S Online supplementary data available from stacks.iop.org/NANO/26/105603/mmedia
GaAs/Al-GaAs core-shell nanowires fabricated by molecular beam epitaxy contain quantum confining structures susceptible of producing narrow photoluminescence (PL) and single photons. The nanoscale chemical mapping of these structures is analyzed in 3D by atom probe tomography (APT). The study allows us to confirm that Al atoms tend to segregate within the AlGaAs shells towards the vertices of the hexagons defining the nanowire cross section. We also find strong alloy fluctuations remaining AlGaAs shell, leading occasionally to the formation of quantum dots (QDs). The PL emission energies predicted in the framework of a 3D effective mass model for a QD analyzed by APT and the PL spectra measured on other nanowires from the same growth batch are consistent within the experimental uncertainties. V C 2014 AIP Publishing LLC.[http://dx.doi.org/10.1063/1.4904952] Epitaxial semiconductor quantum dots (QDs) have been extensively studied over the last three decades because of their peculiar optical properties such as narrow luminescence and single photon emission. The structure and chemical composition of QDs has traditionally been assessed by scanning tunneling microscopy (STM) or transmission electron microscopy (TEM) related techniques. 1 In the last decade, laser-assisted atom probe tomography (LA-APT) 2 has emerged as a tool for the determination of the morphology and of the chemical composition of nanoscale semiconductor heterostructures with sub-nanometer resolution in 3D. 3,4 In the past few years, several APT-based studies addressed a limited number of QD structures. 4-10 Quantum dots can be inserted in semiconductor nanowires either deterministically, with specific shape and composition, 11-14 or as self-assembled structures. [15][16][17][18] Nanowires, furthermore, represent a model system for atom probe analysis, 19-24 as they closely approximate the shape of a field-emission tip. Nevertheless, and despite the interest of nanowire-based QDs for quantum information [25][26][27][28][29] and for their integration in nanoscale optoelectronic devices, [30][31][32][33] no studies of nanowire QDs by APT have been reported yet.Core-shell GaAs/AlGaAs nanowires grown by molecular beam epitaxy (MBE) have been shown to exhibit narrow luminescence and single photon emission, ascribed to QDs forming occasionally at the external corners of the AlGaAs shells. 27 Isolated emissions centered around 670 nm ($1.85 eV) could be found by cathodoluminescence (CL) spectroscopy, with a typical mean frequency along the axis of the order of one spot per micron. 27 Previous studies of these structures performed by highresolution scanning transmission electron microscopy (HR-STEM), electron energy loss spectroscopy (EELS), and energy-dispersive X-ray spectroscopy (EDX) indicated that QDs may form at the outer corner of the hexagon in the AlGaAs shell, at the termination of an Al-segregation region. 27,34 However, it was not possible to fully characterize the shape of the dots nor ascertain whether other mechanisms of QD formation may occ...
This paper describes the fabrication of functional optical devices by sectioning quantum-dot-in-nanowires systems with predefined lengths and orientations. This fabrication process requires only two steps, embedding the nanowires in epoxy and using an ultramicrotome to section them across their axis ("nanoskiving"). This work demonstrates the combination of the following four capabilities: (i) the control of the length of the nanowire sections at the nanometer scale; (ii) the ability to process the nanowires after cutting using wet etching; (iii) the possibility of modifying the geometry of the wire by varying the sectioning angle; and (iv) the generation of as many as 120 consecutive slabs bearing nanowires that have uniform size and approximately reproducible lateral patterns and that can subsequently be transferred to different substrates. The quantum dots inside the nanowires are functional and of a high optical quality after the sectioning process and exhibit photoluminescent emission with wavelengths in the range of 650−710 nm.
Quantum-dot-in-nanowire systems constitute building blocks for advanced photonics and sensing applications. The electronic symmetry of the emitters impacts their function capabilities. Here we study the fine structure of gallium-rich quantum dots nested in the shell of GaAs-Al 0.51 Ga 0.49 As core-shell nanowires. We used optical spectroscopy to resolve the splitting resulting from the exchange terms and extract the main parameters of the emitters. Our results indicate that the quantum dots can host neutral as well as charged excitonic complexes and that the excitons exhibit a slightly elongated footprint, with the main axis tilted with respect to the long axis of the host nanowire. GaAs-Al x Ga 1−x As emitters in a nanowire are particularly promising for overcoming the limitations set by strain in other systems, with the benefit of being integrated in a versatile photonic structure.
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