Sb-saturated high-temperature growth of extended, self-catalyzed GaAsSb nanowires on silicon with high quality.

Ternary GaAsSb nanowires (NW) are key materials for integrated high-speed photonic applications on silicon (Si), where homogeneous, high aspect-ratio dimensions and high-quality properties for controlled absorption, mode confinement and waveguiding are much desired. Here, we demonstrate a unique high-temperature (high-T >650 °C) molecular beam epitaxial (MBE) approach to realize self-catalyzed GaAsSb NWs site-selectively on Si with high aspect-ratio and non-tapered morphologies under antimony (Sb)-saturated conditions. While hitherto reported low-moderate temperature growth processes result in early growth termination and inhomogeneous morphologies, the non-tapered nature of NWs under high-T growth is independent of the supply rates of relevant growth species. Analysis of dedicated Ga-flux and growth time series, allows us to pinpoint the microscopic mechanisms responsible for the elimination of tapering, namely concurrent vapor-solid, step-flow growth along NW side-facets enabled by enhanced Ga diffusion under the high-T growth. Performing growth in an Sb-saturated regime, leads to high Sb-content in VLS-GaAsSb NW close to 30% that is independent of Ga-flux. This independence enables multi-step growth via sequentially increased Ga-flux to realize uniform and very long (>7µm) GaAsSb NWs. The excellent properties of these NWs are confirmed by a completely phase-pure, twin-free zincblende (ZB) crystal structure, a homogeneous Sb-content along the VLS-GaAsSb NW growth axis, along with remarkably narrow, single-peak low-temperature photoluminescence linewidth (<15 meV) at wavelengths of ∼1100-1200 nm.

Wafer-scale epitaxial modulation of quantum dot density.

Precise control of the properties of semiconductor quantum dots (QDs) is vital for creating novel devices for quantum photonics and advanced opto-electronics. Suitable low QD-densities for single QD devices and experiments are challenging to control during epitaxy and are typically found only in limited regions of the wafer. Here, we demonstrate how conventional molecular beam epitaxy (MBE) can be used to modulate the density of optically active QDs in one- and two- dimensional patterns, while still retaining excellent quality. We find that material thickness gradients during layer-by-layer growth result in surface roughness modulations across the whole wafer. Growth on such templates strongly influences the QD nucleation probability. We obtain density modulations between 1 and 10 QDs/µm2 and periods ranging from several millimeters down to at least a few hundred microns. This method is universal and expected to be applicable to a wide variety of different semiconductor material systems. We apply the method to enable growth of ultra-low noise QDs across an entire 3-inch semiconductor wafer.

Ultrathin catalyst-free InAs nanowires on silicon with distinct 1D sub-band transport properties.

Ultrathin InAs nanowires (NW) with a one-dimensional (1D) sub-band structure are promising materials for advanced quantum-electronic devices, where dimensions in the sub-30 nm diameter limit together with post-CMOS integration scenarios on Si are much desired. Here, we demonstrate two site-selective synthesis methods that achieve epitaxial, high aspect ratio InAs NWs on Si with ultrathin diameters below 20 nm. The first approach exploits direct vapor-solid growth to tune the NW diameter by interwire spacing, mask opening size and growth time. The second scheme explores a unique reverse-reaction growth by which the sidewalls of InAs NWs are thermally decomposed under controlled arsenic flux and annealing time. Interesting kinetically limited dependencies between interwire spacing and thinning dynamics are found, yielding diameters as low as 12 nm for sparse NW arrays. We clearly verify the 1D sub-band structure in ultrathin NWs by pronounced conductance steps in low-temperature transport measurements using back-gated NW-field effect transistors. Correlated simulations reveal single- and double degenerate conductance steps, which highlight the rotational hexagonal symmetry and reproduce the experimental traces in the diffusive 1D transport limit. Modelling under the realistic back-gate configuration further evidences regimes that lead to asymmetric carrier distribution and breakdown of the degeneracy depending on the gate bias.

Optical absorption of composition-tunable InGaAs nanowire arrays.

InGaAs nanowire (NW) arrays have emerged as important active materials in future photovoltaic and photodetector applications, due to their excellent electronic properties and tunable band gap. Here, we report a systematic investigation of the optical absorption characteristics of composition-tunable vertical InGaAs NW arrays. Using finite-difference time-domain simulations we first study the effect of variable composition (Ga-molar fraction) and NW array geometry (NW diameter, period, fill factor) on the optical generation rate. NWs with typical diameters in the range of ∼100-250 nm lead to generation rates higher than the equivalent bulk case for moderate fill factors (NW period of ∼0.3-0.8 µm), while slightly smaller fill factors and increased diameters are required to maintain high generation rates at increased Ga-molar fraction. The optical absorption was further measured using spectrally resolved ultraviolet-visible-near-infrared (UV-vis-NIR) spectroscopy on NW arrays transferred to transparent substrates. Interestingly, large variations in Ga-molar fraction (0 < x(Ga) < 0.5) have a negligible influence, while minute changes in NW diameter of less than ±20 nm affect the absorption spectra very strongly, leading to pronounced shifts in the peak absorption energies by more than ∼700 meV. These results clearly highlight the much larger sensitivity of the optical absorption behavior to geometric parameters rather than to variations in the electronic band gap of the underlying NW array.

Site-selectively generated photon emitters in monolayer MoS2 via local helium ion irradiation.

Quantum light sources in solid-state systems are of major interest as a basic ingredient for integrated quantum photonic technologies. The ability to tailor quantum emitters via site-selective defect engineering is essential for realizing scalable architectures. However, a major difficulty is that defects need to be controllably positioned within the material. Here, we overcome this challenge by controllably irradiating monolayer MoS2 using a sub-nm focused helium ion beam to deterministically create defects. Subsequent encapsulation of the ion exposed MoS2 flake with high-quality hBN reveals spectrally narrow emission lines that produce photons in the visible spectral range. Based on ab-initio calculations we interpret these emission lines as stemming from the recombination of highly localized electron-hole complexes at defect states generated by the local helium ion exposure. Our approach to deterministically write optically active defect states in a single transition metal dichalcogenide layer provides a platform for realizing exotic many-body systems, including coupled single-photon sources and interacting exciton lattices that may allow the exploration of Hubbard physics.

Tuning Lasing Emission toward Long Wavelengths in GaAs-(In,Al)GaAs Core-Multishell Nanowires.

Semiconductor nanowire (NW) lasers are attractive as integrated on-chip coherent light sources with strong potential for applications in optical communication and sensing. Realizing lasers from individual bulk-type NWs with emission tunable from the near-infrared to the telecommunications spectral region is, however, challenging and requires low-dimensional active gain regions with an adjustable band gap and quantum confinement. Here, we demonstrate lasing from GaAs-(InGaAs/AlGaAs) core-shell NWs with multiple InGaAs quantum wells (QW) and lasing wavelengths tunable from ∼0.8 to ∼1.1 µm. Our investigation emphasizes particularly the critical interplay between QW design, growth kinetics, and the control of InGaAs composition in the active region needed for effective tuning of the lasing wavelength. A low shell growth temperature and GaAs interlayers at the QW/barrier interfaces enable In molar fractions up to ∼25% without plastic strain relaxation or alloy intermixing in the QWs. Correlated scanning transmission electron microscopy, atom probe tomography, and confocal PL spectroscopy analyses illustrate the high sensitivity of the optically pumped lasing characteristics on microscopic properties, providing useful guidelines for other III-V-based NW laser systems.

Coupling Single Photons from Discrete Quantum Emitters in WSe2 to Lithographically Defined Plasmonic Slot Waveguides.

We report the observation of the generation and routing of single plasmons generated by localized excitons in a WSe2 monolayer flake exfoliated onto lithographically defined Au-plasmonic waveguides. Statistical analysis of the position of different quantum emitters shows that they are (3.3 ± 0.7) times more likely to form close to the edges of the plasmonic waveguides. By characterizing individual emitters, we confirm their single-photon character via the observation of antibunching in the signal ( g(2)(0) = 0.42) and demonstrate that specific emitters couple to modes of the proximal plasmonic waveguide. Time-resolved measurements performed on emitters close to and far away from the plasmonic nanostructures indicate that Purcell factors up to 15 ± 3 occur, depending on the precise location of the quantum emitter relative to the tightly confined plasmonic mode. Measurement of the point spread function of five quantum emitters relative to the waveguide with <50 nm precision is compared with numerical simulations to demonstrate the potential for greater increases in the coupling efficiency for ideally positioned emitters. The integration of such strain-induced quantum emitters with deterministic plasmonic routing is a step toward deep-subwavelength on-chip single quantum light sources.

A few-emitter solid-state multi-exciton laser.

We report on non-conventional lasing in a photonic-crystal nanocavity that operates with only four solid-state quantum-dot emitters. In a comparison between microscopic theory and experiment, we demonstrate that irrespective of emitter detuning, lasing with [Formula: see text] is facilitated by means of emission from dense-lying multi-exciton states. In the spontaneous-emission regime we find signatures for radiative coupling between the quantum dots. The realization of different multi-exciton states at different excitation powers and the presence of electronic inter-emitter correlations are reflected in a pump-rate dependence of the ß-factor.

Long-term mutual phase locking of picosecond pulse pairs generated by a semiconductor nanowire laser.

The ability to generate phase-stabilized trains of ultrafast laser pulses by mode-locking underpins photonics research in fields, such as precision metrology and spectroscopy. However, the complexity of conventional mode-locked laser systems has hindered their realization at the nanoscale. Here we demonstrate that GaAs-AlGaAs nanowire lasers are capable of emitting pairs of phase-locked picosecond laser pulses with a repetition frequency up to 200 GHz when subject to incoherent pulsed optical excitation. By probing the two-pulse interference spectra, we show that pulse pairs remain mutually coherent over timescales extending to 30 ps, much longer than the emitted laser pulse duration (≤3 ps). Simulations performed by solving the optical Bloch equations produce good quantitative agreement with experiments, revealing how the phase information is stored in the gain medium close to transparency. Our results open the way to phase locking of nanowires integrated onto photonic circuits, optical injection locking and applications, such as on-chip Ramsey comb spectroscopy.

Electric-Field Switchable Second-Harmonic Generation in Bilayer MoS2 by Inversion Symmetry Breaking.

We demonstrate pronounced electric-field-induced second-harmonic generation in naturally inversion symmetric 2H stacked bilayer MoS2 embedded into microcapacitor devices. By applying strong external electric field perturbations (|F| = ±2.6 MV cm-1) perpendicular to the basal plane of the crystal, we control the inversion symmetry breaking and, hereby, tune the nonlinear conversion efficiency. Strong tunability of the nonlinear response is observed throughout the energy range (Eω ∼ 1.25-1.47 eV) probed by measuring the second-harmonic response at E2ω, spectrally detuned from both the A- and B-exciton resonances. A 60-fold enhancement of the second-order nonlinear signal is obtained for emission at E2ω = 2.49 eV, energetically detuned by ΔE = E2ω - EC = -0.26 eV from the C-resonance (EC = 2.75 eV). The pronounced spectral dependence of the electric-field-induced second-harmonic generation signal reflects the bandstructure and wave function admixture and exhibits particularly strong tunability below the C-resonance, in good agreement with density functional theory calculations. Moreover, we show that the field-induced second-harmonic generation relies on the interlayer coupling in the bilayer. Our findings strongly suggest that the strong tunability of the electric-field-induced second-harmonic generation signal in bilayer transition metal dichalcogenides may find applications in miniaturized electrically switchable nonlinear devices.

Quantum Effects in Higher-Order Correlators of a Quantum-Dot Spin Qubit.

We measure time correlators of a spin qubit in an optically active quantum dot beyond the second order. Such higher-order correlators are shown to be directly sensitive to pure quantum effects that cannot be explained within the classical framework. They allow direct determination of ensemble and quantum dephasing times, T_{2}^{*} and T_{2}, using only repeated projective measurements and without the need for coherent spin control. Our method enables studies of purely quantum behavior in solid state systems, including tests of the Leggett-Garg type of inequalities that rule out local hidden variable interpretation of the quantum-dot spin dynamics.

Surface plasmon resonance spectroscopy of single bowtie nano-antennas using a differential reflectivity method.

We report on the structural and optical properties of individual bowtie nanoantennas both on glass and semiconducting GaAs substrates. The antennas on glass (GaAs) are shown to be of excellent quality and high uniformity reflected by narrow size distributions with standard deviations for the triangle and gap size of = 4.5 nm = 2.6 nm and = 5.4 nm = 3.8 nm, respectively. The corresponding optical properties of individual nanoantennas studied by differential reflection spectroscopy show a strong reduction of the localised surface plasmon polariton resonance linewidth from 0.21 eV to 0.07 eV upon reducing the antenna size from 150 nm to 100 nm. This is attributed to the absence of inhomogeneous broadening as compared to optical measurements on nanoantenna ensembles. The inter-particle coupling of an individual bowtie nanoantenna, which gives rise to strongly localised and enhanced electromagnetic hotspots, is demonstrated using polarization-resolved spectroscopy, yielding a large degree of linear polarization of ρmax ~ 80%. The combination of highly reproducible nanofabrication and fast, non-destructive and non-contaminating optical spectroscopy paves the route towards future semiconductor-based nano-plasmonic circuits, consisting of multiple photonic and plasmonic entities.

Coulomb Mediated Hybridization of Excitons in Coupled Quantum Dots.

We report Coulomb mediated hybridization of excitonic states in optically active InGaAs quantum dot molecules. By probing the optical response of an individual quantum dot molecule as a function of the static electric field applied along the molecular axis, we observe unexpected avoided level crossings that do not arise from the dominant single-particle tunnel coupling. We identify a new few-particle coupling mechanism stemming from Coulomb interactions between different neutral exciton states. Such Coulomb resonances hybridize the exciton wave function over four different electron and hole single-particle orbitals. Comparisons of experimental observations with microscopic eight-band k·p calculations taking into account a realistic quantum dot geometry show good agreement and reveal that the Coulomb resonances arise from broken symmetry in the artificial semiconductor molecule.

Stark Effect Spectroscopy of Mono- and Few-Layer MoS2.

We demonstrate electrical control of the A-exciton interband transition in mono- and few-layer MoS2 crystals embedded into photocapacitor devices via the DC Stark effect. Electric field-dependent low-temperature photoluminescence spectroscopy reveals a significant tuneability of the A-exciton transition energy up to ∼ 16 meV from which we extract the mean DC exciton polarizability ⟨ß̅N⟩ = (0.58 ± 0.25) × 10(-8) Dm V(-1). The exciton polarizability is shown to be layer-independent, indicating a strong localization of both electron and hole wave functions in each individual layer.

Monolithically Integrated High-ß Nanowire Lasers on Silicon.

Reliable technologies for the monolithic integration of lasers onto silicon represent the holy grail for chip-level optical interconnects. In this context, nanowires (NWs) fabricated using III-V semiconductors are of strong interest since they can be grown site-selectively on silicon using conventional epitaxial approaches. Their unique one-dimensional structure and high refractive index naturally facilitate low loss optical waveguiding and optical recirculation in the active NW-core region. However, lasing from NWs on silicon has not been achieved to date, due to the poor modal reflectivity at the NW-silicon interface. We demonstrate how, by inserting a tailored dielectric interlayer at the NW-Si interface, low-threshold single mode lasing can be achieved in vertical-cavity GaAs-AlGaAs core-shell NW lasers on silicon as measured at low temperature. By exploring the output characteristics along a detection direction parallel to the NW-axis, we measure very high spontaneous emission factors comparable to nanocavity lasers (ß = 0.2) and achieve ultralow threshold pump energies ≤11 pJ/pulse. Analysis of the input-output characteristics of the NW lasers and the power dependence of the lasing emission line width demonstrate the potential for high pulsation rates ≥250 GHz. Such highly efficient nanolasers grown monolithically on silicon are highly promising for the realization of chip-level optical interconnects.

Ultrafast Photodetection in the Quantum Wells of Single AlGaAs/GaAs-Based Nanowires.

We investigate the ultrafast optoelectronic properties of single Al0.3Ga0.7As/GaAs core-shell nanowires. The nanowires contain GaAs-based quantum wells. For a resonant excitation of the quantum wells, we find a picosecond photocurrent which is consistent with an ultrafast lateral expansion of the photogenerated charge carriers. This Dember-effect does not occur for an excitation of the GaAs-based core of the nanowires. Instead, the core exhibits an ultrafast displacement current and a photothermoelectric current at the metal Schottky contacts. Our results uncover the optoelectronic dynamics in semiconductor core-shell nanowires comprising quantum wells, and they demonstrate the possibility to use the low-dimensional quantum well states therein for ultrafast photoswitches and photodetectors.

On-Chip Generation, Routing, and Detection of Resonance Fluorescence.

Quantum optical circuits can be used to generate, manipulate, and exploit nonclassical states of light to push semiconductor based photonic information technologies to the quantum limit. Here, we report the on-chip generation of quantum light from individual, resonantly excited self-assembled InGaAs quantum dots, efficient routing over length scales ≥1 mm via GaAs ridge waveguides, and in situ detection using evanescently coupled integrated NbN superconducting single photon detectors fabricated on the same chip. By temporally filtering the time-resolved luminescence signal stemming from single quantum dots we use the quantum optical circuit to perform time-resolved excitation spectroscopy on single dots and demonstrate resonance fluorescence with a line-width of 10 ± 1 µeV; key elements needed for the use of single photons in prototypical quantum photonic circuits.

Demonstration of Confined Electron Gas and Steep-Slope Behavior in Delta-Doped GaAs-AlGaAs Core-Shell Nanowire Transistors.

Strong surface and impurity scattering in III-V semiconductor-based nanowires (NW) degrade the performance of electronic devices, requiring refined concepts for controlling charge carrier conductivity. Here, we demonstrate remote Si delta (δ)-doping of radial GaAs-AlGaAs core-shell NWs that unambiguously exhibit a strongly confined electron gas with enhanced low-temperature field-effect mobilities up to 5 × 10(3) cm(2) V(-1) s(-1). The spatial separation between the high-mobility free electron gas at the NW core-shell interface and the Si dopants in the shell is directly verified by atom probe tomographic (APT) analysis, band-profile calculations, and transport characterization in advanced field-effect transistor (FET) geometries, demonstrating powerful control over the free electron gas density and conductivity. Multigated NW-FETs allow us to spatially resolve channel width- and crystal phase-dependent variations in electron gas density and mobility along single NW-FETs. Notably, dc output and transfer characteristics of these n-type depletion mode NW-FETs reveal excellent drain current saturation and record low subthreshold slopes of 70 mV/dec at on/off ratios >10(4)-10(5) at room temperature.

Emitters of N-photon bundles.

Controlling the ouput of a light emitter is one of the basic tasks of photonics, with landmarks such as the laser and single-photon sources. The development of quantum applications makes it increasingly important to diversify the available quantum sources. Here, we propose a cavity QED scheme to realize emitters that release their energy in groups, or "bundles" of N photons, for integer N. Close to 100% of two-photon emission and 90% of three-photon emission is shown to be within reach of state of the art samples. The emission can be tuned with system parameters so that the device behaves as a laser or as a N-photon gun. The theoretical formalism to characterize such emitters is developed, with the bundle statistics arising as an extension of the fundamental correlation functions of quantum optics. These emitters will be useful for quantum information processing and for medical applications.

Optical study of lithographically defined, subwavelength plasmonic wires and their coupling to embedded quantum emitters.

We present an optical investigation of surface plasmon polaritons propagating along nanoscale Au-wires, lithographically defined on GaAs substrates. A two-axis confocal microscope was used to perform spatially and polarization resolved measurements in order to confirm the guiding of surface plasmon polaritons over lengths ranging from 5 to 20 µm along nanowires with a lateral dimension of only ≈ 100 nm. Finite difference time domain simulations are used to corroborate our experimental observations, and highlight the potential to couple proximal quantum emitters to propagating plasmon modes in such extreme subwavelength devices. Our findings are of strong relevance for the development of semiconductor based integrated plasmonic and active quantum plasmonic nanosystems that merge quantum emitters with nanoscale plasmonic elements.