Annealing-Modulated Surface Reconstruction for Self-Assembly of High-Density Uniform InAs/GaAs Quantum Dots on Large Wafers Substrate.

In this work, we developed pre-grown annealing to form ß2 reconstruction sites among ß or α (2 × 4) reconstruction phase to promote nucleation for high-density, size/wafer-uniform, photoluminescence (PL)-optimal InAs quantum dot (QD) growth on a large GaAs wafer. Using this, the QD density reached 580 (860) µm-2 at a room-temperature (T) spectral FWHM of 34 (41) meV at the wafer center (and surrounding) (high-rate low-T growth). The smallest FWHM reached 23.6 (24.9) meV at a density of 190 (260) µm-2 (low-rate high-T). The mediate rate formed uniform QDs in the traditional ß phase, at a density of 320 (400) µm-2 and a spectral FWHM of 28 (34) meV, while size-diverse QDs formed in ß2 at a spectral FWHM of 92 (68) meV and a density of 370 (440) µm-2. From atomic-force-microscope QD height distribution and T-dependent PL spectroscopy, it is found that compared to the dense QDs grown in ß phase (mediate rate, 320 µm-2) with the most large dots (240 µm-2), the dense QDs grown in ß2 phase (580 µm-2) show many small dots with inter-dot coupling in favor of unsaturated filling and high injection to large dots for PL. The controllable annealing (T, duration) forms ß2 or ß2-mixed α or ß phase in favor of a wafer-uniform dot island and the faster T change enables optimal T for QD growth.

Single- and Twin-Photons Emitted from Fiber-Coupled Quantum Dots in a Distributed Bragg Reflector Cavity.

In this work, we develop single-mode fiber devices of an InAs/GaAs quantum dot (QD) by bonding a fiber array with large smooth facet, small core, and small numerical aperture to QDs in a distributed Bragg reflector planar cavity with vertical light extraction that prove mode overlap and efficient output for plug-and-play stable use and extensive study. Modulated Si doping as electron reservoir builds electric field and level tunnel coupling to reduce fine-structure splitting (FSS) and populate dominant XX and higher excitons XX+ and XXX. Epoxy package thermal stress induces light hole (lh) with various behaviors related to the donor field: lh h1 confined with more anisotropy shows an additional XZ line (its space to the traditional X lines reflects the field intensity) and larger FSS; lh h2 delocalized to wetting layer shows a fast h2-h1 decay; lh h2 confined shows D3h symmetric higher excitons with slow h2-h1 decay and more confined h1 to raise h1-h1 Coulomb interaction.

Tailoring solid-state single-photon sources with stimulated emissions.

The coherent interaction of electromagnetic fields with solid-state two-level systems can yield deterministic quantum light sources for photonic quantum technologies. To date, the performance of semiconductor single-photon sources based on three-level systems is limited mainly due to a lack of high photon indistinguishability. Here we tailor the cavity-enhanced spontaneous emission from a ladder-type three-level system in a single epitaxial quantum dot through stimulated emission. After populating the biexciton (XX) of the quantum dot through two-photon resonant excitation, we use another laser pulse to selectively depopulate the XX state into an exciton (X) state with a predefined polarization. The stimulated XX-X emission modifies the X decay dynamics and improves the characteristics of a polarized single-photon source, such as a source brightness of 0.030(2), a single-photon purity of 0.998(1) and an indistinguishability of 0.926(4). Our method can be readily applied to existing quantum dot single-photon sources and expands the capabilities of three-level systems for advanced quantum photonic functionalities.

Wet-Etched Microlens Array for 200 nm Spatial Isolation of Epitaxial Single QDs and 80 nm Broadband Enhancement of Their Quantum Light Extraction.

Uniform arrays of three shapes (gauss, hat, and peak) of GaAs microlenses (MLs) by wet-etching are demonstrated, ∼200 nm spatial isolation of epitaxial single QDs embedded (λ: 890-990 nm) and broadband (Δλ∼80 nm) enhancement of their quantum light extraction are obtained, which is also suitable for telecom-band epitaxial QDs. Combined with the bottom distributed Bragg reflector, the hat-shaped ML forms a cavity and achieves the best enhancement: extraction efficiency of 26%, Purcell factor of 2 and single-photon count rate of 7×106 counts per second at the first lens; while the gauss-shaped ML shows a broader band (e.g., longer λ) enhancement. In the MLs, single QDs with featured exciton emissions are observed, whose time correlations prove single-photon emission with multi-photon probability g(2)(0)=0.02; some QDs show both biexciton XX and exciton X emissions and exhibit a perfect cascade feature. This work could pave a step towards a scalable array of QD single-photon sources and the application of QD photon-pair emission for entanglement experiments.

Boost of single-photon emission by perfect coupling of InAs/GaAs quantum dot and micropillar cavity mode.

We proposed a precise calibration process of Al 0.9Ga0.1As/GaAs DBR micropillar cavity to match the single InAs/GaAs quantum dot (QD) exciton emission and achieve cavity mode resonance and a great enhancement of QD photoluminescence (PL) intensity. Light-matter interaction of single QD in DBR micropillar cavity (Q ∼ 3800) under weak coupling regime was investigated by temperature-tuned PL spectra; a pronounced enhancement (14.6-fold) of QD exciton emission was observed on resonance. The second-order autocorrelation measurement shows g(2)(0)=0.070, and the estimated net count rate before the first objective lens reaches 1.6×107 counts/s under continuous wave excitation, indicating highly pure single-photon emission at high count rates.

Bright Single-Photon Source at 1.3 µm Based on InAs Bilayer Quantum Dot in Micropillar.

A pronounced high count rate of single-photon emission at the wavelength of 1.3 µm that is capable of fiber-based quantum communication from InAs/GaAs bilayer quantum dots coupled with a micropillar (diameter ~3 µm) cavity of distributed Bragg reflectors was investigated, whose photon extraction efficiency has achieved 3.3%. Cavity mode and Purcell enhancement have been observed clearly in microphotoluminescence spectra. At the detection end of Hanbury-Brown and Twiss setup, the two avalanched single-photon counting modules record a total count rate of ~62,000/s; the time coincidence counting measurement demonstrates single-photon emission, with the multi-photon emission possibility, i.e., g 2(0), of only 0.14.

Large optical Stark shifts in single quantum dots coupled to core-shell GaAs/AlGaAs nanowires.

Nanowire quantum dots (NW-QDs) can be used for future compact and efficient optoelectronic devices. Many efforts have been made to control the QD states by inserting the QDs in doped structures and applying an electric field in a nanowire system. In this paper, we use down-conversion and up-conversion photoluminescence excitations to explore the optical and electronic properties of single quantum dots in GaAs/AlGaAs core-shell nanowires. We investigate a large optical Stark shift in this system as a new method to tune the QD states. When the tunable laser lies within the spectral bandwidth of ZB/WZ GaAs (780 nm-860 nm), we observe an extremely large optical Stark shift of 1.3 nm (0.5 nm) with increasing excitation power at a resonant wavelength of 800 nm (840 nm) in GaAs states. The ability to in situ control the energy states of self-catalyzed NW-QDs should open a new way for quantum light sources and nonlinear optics in a nanowire system.

Telecommunication Wavelength-Band Single-Photon Emission from Single Large InAs Quantum Dots Nucleated on Low-Density Seed Quantum Dots.

Single-photon emission in the telecommunication wavelength band is realized with self-assembled strain-coupled bilayer InAs quantum dots (QDs) embedded in a planar microcavity on GaAs substrate. Low-density large QDs in the upper layer active for ~1.3 µm emission are fabricated by precisely controlling the indium deposition amount and applying a gradient indium flux in both QD layers. Time-resolved photoluminescence (PL) intensity suggested that the radiative lifetime of their exciton emission is 1.5~1.6 ns. The second-order correlation function of g (2)(0) < 0.5 which demonstrates a pure single-photon emission.

In situ probing and integration of single self-assembled quantum dots-in-nanowires for quantum photonics.

The realization of fiber-output single photon sources is necessary for quantum photonics. Here we present in situ probing and integration of single self-assembled quantum dots (QDs)-in-nanowires. Single self-assembled AlGaAs QDs were synthesized in GaAs/AlGaAs core-shell nanowires by molecular beam epitaxy and characterized by optical excitation in both micro-PL and fiber-integrating set-up. Cascaded biexciton-exciton emission with a saturation signal of 1000 counts per second at nitrogen temperature is achieved through the fiber-integrating setup, which makes single mode fibers an ideal candidate for single photons sources and paves the way for the realization of 'all fiber' devices. Numerical calculations were carried out to illustrate the collection efficiency and polarized photoluminescence characteristics. Extraction efficiencies as high as 70% over a broadband emission are reported and increase by a factor of about seven in comparison with air extraction, due to the larger refractive index of the fiber core.

Morphological engineering of self-assembled nanostructures at nanoscale on faceted GaAs nanowires by droplet epitaxy.

Fabrication of advanced artificial nanomaterials is a long-term pursuit to fulfill the promises of nanomaterials and it is of utter importance to manipulate materials at nanoscale to meet urgent demands of nanostructures with designed properties. Herein, we demonstrate the morphological tailoring of self-assembled nanostructures on faceted GaAs nanowires (NWs). The NWs are deposited on different kinds of substrates. Triangular and hexagonal prism morphologies are obtained, and their corresponding {110} sidewalls act as platforms for the nucleation of gallium droplets (GDs). We demonstrate that the morphologies of the nanostructures depend not only on the annealing conditions but also on the morphologies of the NWs' sidewalls. Here, we achieve morphological engineering in the form of novel quantum dots (QDs), 'square' quantum rings (QRs), 'rectangular' QRs, 3D QRs, crescent-shaped QRs, and nano-antidots. The evolution mechanisms for the peculiar morphologies of both NWs and nanostructures are modeled and discussed in detail. This work shows the potential of combining nano-structural engineering with NWs to achieve multifunctional properties and applications.

Self-assembled quantum dot structures in a hexagonal nanowire for quantum photonics.

Two types of quantum nanostructures based on self-assembled GaAs quantumdots embedded into GaAs/AlGaAs hexagonal nanowire systems are reported, opening a new avenue to the fabrication of highly efficient single-photon sources, as well as the design of novel quantum optics experiments and robust quantum optoelectronic devices operating at higher temperature, which are required for practical quantum photonics applications.

Self-assembly of single "square" quantum rings in gold-free GaAs nanowires.

Single nanostructures embedded within nanowires (NWs) represent one of the most promising technologies for applications in quantum photonics. However, fabrication imperfections and etching-induced defects are inevitable for top-down fabrications, whereas self-assembly bottom-up approaches cannot avoid the difficulties of its stochastic nature and are limited to restricted heterogeneous material systems. Here we demonstrate the versatile self-assembly of single "square" quantum rings (QR) on the sidewalls of gold-free GaAs NWs for the first time. By tuning the deposition temperature, As overpressure and amount of gallium-droplets, we were able to control the density and morphology of the structure, yielding novel single quantum dots, QR, coupled QRs, and nano-antidots. A proposed model based on a strain-driven, transport-dependent nucleation of gallium droplets at high temperature accounts for the formation mechanism of these structures. We achieved a single-QR-in-NW structure, of which the optical properties were analyzed using micro-photoluminescence at 10 K and a spatially resolved cathodoluminescence technique at 77 K. The spectra show sharp discrete peaks; of these peaks, the narrowest linewidth (separation) was 578 µeV (1-3 meV), reflecting the quantized nature of the ring-type electronic states.

Single InAs quantum dot grown at the junction of branched gold-free GaAs nanowire.

We report a new type of single InAs quantum dot (QD) embedded at the junction of gold-free branched GaAs/AlGaAs nanowire (NW) grown on silicon substrate. The photoluminescence intensity of such QD is ~20 times stronger than that from randomly distributed QD grown on the facet of straight NW. Sharp excitonic emission is observed at 4.2 K with a line width of 101 µeV and a vanishing two-photon emission probability of g(2)(0) = 0.031(2). This new nanostructure may open new ways for designing novel quantum optoelectronic devices.

In situ accurate control of 2D-3D transition parameters for growth of low-density InAs/GaAs self-assembled quantum dots.

A method to improve the growth repeatability of low-density InAs/GaAs self-assembled quantum dots by molecular beam epitaxy is reported. A sacrificed InAs layer was deposited firstly to determine in situ the accurate parameters of two- to three-dimensional transitions by observation of reflection high-energy electron diffraction patterns, and then the InAs layer annealed immediately before the growth of the low-density InAs quantum dots (QDs). It is confirmed by micro-photoluminescence that control repeatability of low-density QD growth is improved averagely to about 80% which is much higher than that of the QD samples without using a sacrificed InAs layer.