Optical net gain measurement on Al0.07Ga0.93N/GaN multi-quantum wells.

We report net gain measurements at room temperature in Al0.07Ga0.93N/GaN 10-period multi-quantum well layers emitting at 367 nm, using the variable stripe length method. The separate confinement heterostructure was designed targeting electron-beam pumped lasing at 10 kV. The highest net gain value was 131 cm-1, obtained at the maximum pumping power density of the experimental setup (743 kW/cm2). The net gain threshold was attained at 218 kW/cm2 using 193 nm optical pumping. From these experiments, we predict an electron-beam-pumped lasing threshold of 370 kW/cm2 at room temperature, which is compatible with the use of compact cathodes (e.g. carbon nanotubes). In some areas of the sample, we observed an anomalous amplification of the photoluminescence intensity that occurs for long stripe lengths (superior to 400 µm) and high pumping power (superior to 550 kW/cm2), leading to an overestimation of the net gain value. We attribute such a phenomenon to the optical feedback provided by the reflection from cracks, which were created during the epitaxial growth due to the strong lattice mismatch between different layers.

Room-Temperature Doping of CsPbBr3 Nanocrystals with Aluminum.

B-site doping is an emerging strategy for tuning the emission wavelength of cesium lead halide ABX3 nanocrystals. We present a simple method for the postsynthetic doping of CsPbBr3 nanocrystals with aluminum at room temperature by exposing them to a solution of AlBr3 in dibromomethane. Despite the much smaller ionic radius of Al3+ compared to that of Pb2+, nominal doping levels in a range from 8.1% to 24.3% were obtained when increasing the Al/Pb feed ratio from 1 to 4.5. Al3+ introduction leads to a hypsochromic shift of the photoluminescence (PL) emission of the CsPbBr3 nanocrystals. The PL peak position is highly stable over at least 6 months and tunable in a range of 510 to 480 nm by increasing the doping level. Structural analyses revealed a linear correlation between the PL energy and the lattice parameter with a slope of -1.96 eV/Å.

AlGaN/GaN asymmetric graded-index separate confinement heterostructures designed for electron-beam pumped UV lasers.

We present a study of undoped AlGaN/GaN separate confinement heterostructures designed to operate as electron beam pumped ultraviolet lasers. We discuss the effect of spontaneous and piezoelectric polarization on carrier diffusion, comparing the results of cathodoluminescence with electronic simulations of the band structure and Monte Carlo calculations of the electron trajectories. Carrier collection is significantly improved using an asymmetric graded-index separate confinement heterostructure (GRINSCH). The graded layers avoid potential barriers induced by polarization differences in the heterostructure and serve as strain transition buffers which reduce the mosaicity of the active region and the linewidth of spontaneous emission.

Light Controlled Optical Aharonov-Bohm Oscillations in a Single Quantum Ring.

We found that optical Aharonov-Bohm oscillations in a single GaAs/GaAlAs quantum ring can be controlled by excitation intensity. With a weak excitation intensity of 1.2 kW cm-2, the optical Aharonov-Bohm oscillation period of biexcitons was observed to be half that of excitons in accordance with the period expected for a two-exciton Wigner molecule. When the excitation intensity is increased by an order of magnitude (12 kW cm-2), a gradual deviation of the Wigner molecule condition occurs with decreased oscillation periods and diamagnetic coefficients for both excitons and biexcitons along with a spectral shift. These results suggest that the effective orbit radii and rim widths of electrons and holes in a single quantum ring can be modified by light intensity via photoexcited carriers, which are possibly trapped at interface defects resulting in a local electric field.

Quasi-one-dimensional density of states in a single quantum ring.

Generally confinement size is considered to determine the dimensionality of nanostructures. While the exciton Bohr radius is used as a criterion to define either weak or strong confinement in optical experiments, the binding energy of confined excitons is difficult to measure experimentally. One alternative is to use the temperature dependence of the radiative recombination time, which has been employed previously in quantum wells and quantum wires. A one-dimensional loop structure is often assumed to model quantum rings, but this approximation ceases to be valid when the rim width becomes comparable to the ring radius. We have evaluated the density of states in a single quantum ring by measuring the temperature dependence of the radiative recombination of excitons, where the photoluminescence decay time as a function of temperature was calibrated by using the low temperature integrated intensity and linewidth. We conclude that the quasi-continuous finely-spaced levels arising from the rotation energy give rise to a quasi-one-dimensional density of states, as long as the confined exciton is allowed to rotate around the opening of the anisotropic ring structure, which has a finite rim width.

Exciton Dipole-Dipole Interaction in a Single Coupled-Quantum-Dot Structure via Polarized Excitation.

We find that the exciton dipole-dipole interaction in a single laterally coupled GaAs/AlGaAs quantum dot structure can be controlled by the linear polarization of a nonresonant optical excitation. When the excitation intensity is increased with the linearly polarized light parallel to the lateral coupling direction [11̅0], excitons (X1 and X2) and local biexcitons (X1X1 and X2X2) of the two separate quantum dots (QD1 and QD2) show a redshift along with coupled biexcitons (X1X2), while neither coupled biexcitons nor a redshift are observed when the polarization of the exciting beam is perpendicular to the coupling direction. The polarization dependence and the redshift are attributed to an optical nonlinearity in the exciton Förster resonant energy transfer interaction, whereby exciton population transfer between the two quantum dots also becomes significant with increasing excitation intensity. We have further distinguished coupled biexcitons from local biexcitons by their large diamagnetic coefficient.

Determination of the Optimal Shell Thickness for Self-Catalyzed GaAs/AlGaAs Core-Shell Nanowires on Silicon.

We present a set of experimental results showing a combination of various effects, that is, surface recombination velocity, surface charge traps, strain, and structural defects, that govern the carrier dynamics of self-catalyzed GaAs/AlGaAs core-shell nanowires (NWs) grown on a Si(111) substrate by molecular beam epitaxy. Time-resolved photoluminescence of NW ensemble and spatially resolved cathodoluminescence of single NWs reveal that emission intensity, decay time, and carrier diffusion length of the GaAs NW core strongly depend on the AlGaAs shell thickness but in a nonmonotonic fashion. Although 7 nm AlGaAs shell can efficiently suppress the surface recombination velocity of the GaAs NW core, the influence of the surface charge traps and the strain between the core and the shell that redshift the luminescence of the GaAs NW core remain observable in the whole range of the shell thickness. In addition, the band bending effect induced by the surface charge traps can alter the scattering of the excess carriers inside the GaAs NW core at the core/shell interface. If the AlGaAs shell thickness is larger than 50 nm, the luminescence efficiency of the GaAs NW cores deteriorates, ascribed to defect formation inside the AlGaAs shell evidenced by transmission electron microscopy.

Observation of a Biexciton Wigner Molecule by Fractional Optical Aharonov-Bohm Oscillations in a Single Quantum Ring.

The Aharonov-Bohm effect in ring structures in the presence of electronic correlation and disorder is an open issue. We report novel oscillations of a strongly correlated exciton pair, similar to a Wigner molecule, in a single nanoquantum ring, where the emission energy changes abruptly at the transition magnetic field with a fractional oscillation period compared to that of the exciton, a so-called fractional optical Aharonov-Bohm oscillation. We have also observed modulated optical Aharonov-Bohm oscillations of an electron-hole pair and an anticrossing of the photoluminescence spectrum at the transition magnetic field, which are associated with disorder effects such as localization, built-in electric field, and impurities.

Self-aligned deterministic coupling of single quantum emitter to nanofocused plasmonic modes.

The quantum plasmonics field has emerged and been growing increasingly, including study of single emitter-light coupling using plasmonic system and scalable quantum plasmonic circuit. This offers opportunity for the quantum control of light with compact device footprint. However, coupling of a single emitter to highly localized plasmonic mode with nanoscale precision remains an important challenge. Today, the spatial overlap between metallic structure and single emitter mostly relies either on chance or on advanced nanopositioning control. Here, we demonstrate deterministic coupling between three-dimensionally nanofocused plasmonic modes and single quantum dots (QDs) without any positioning for single QDs. By depositing a thin silver layer on a site-controlled pyramid QD wafer, three-dimensional plasmonic nanofocusing on each QD at the pyramid apex is geometrically achieved through the silver-coated pyramid facets. Enhancement of the QD spontaneous emission rate as high as 22 ± 16 is measured for all processed QDs emitting over ∼150-meV spectral range. This approach could apply to high fabrication yield on-chip devices for wide application fields, e.g., high-efficiency light-emitting devices and quantum information processing.

Exciton scattering mechanism in a single semiconducting MgZnO nanorod.

Excitonic phenomena, such as excitonic absorption and emission, have been used in many photonic and optoelectronic semiconductor device applications. As the sizes of these nanoscale materials have approached to exciton diffusion lengths in semiconductors, a fundamental understanding of exciton transport in semiconductors has become imperative. We present exciton transport in a single MgZnO nanorod in the spatiotemporal regime with several nanometer-scale spatial resolution and several tens of picosecond temporal resolution. This study was performed using temperature-dependent cathodoluminescence and time-resolved photoluminescence spectroscopies. The exciton diffusion length in the MgZnO nanorod decreased from 100 to 70 nm with increasing temperature in the range of 5 and 80 K. The results obtained for the temperature dependence of exciton diffusion length and luminescence lifetime revealed that the dominant exciton scattering mechanism in MgZnO nanorod is exciton-phonon assisted piezoelectric field scattering.

Carrier depletion and exciton diffusion in a single ZnO nanowire.

Carrier depletion and transport in a single ZnO nanowire Schottky device have been investigated at 5 K, using cathodoluminescence measurements. An exciton diffusion length of 200 nm has been determined along the nanowire axis. The depletion width is found to increase linearly with the reverse bias. The origin of this unusual dependence in semiconductor material is discussed in terms of charge location and dimensional effects on the screening of the junction electric field.

Submicrometre resolved optical characterization of green nanowire-based light emitting diodes.

The electroluminescent properties of InGaN/GaN nanowire-based light emitting diodes (LEDs) are studied at different resolution scales. Axial one-dimensional heterostructures were grown by plasma-assisted molecular beam epitaxy (PAMBE) directly on a silicon (111) substrate and consist of the following sequentially deposited layers: n-type GaN, three undoped InGaN/GaN quantum wells, p-type AlGaN electron blocking layer and p-type GaN. From the macroscopic point of view, the devices emit light in the green spectral range (around 550 nm) under electrical injection. At 100 mA DC current, a 1 mm2 chip that integrates around 10(7) nanowires emits an output power on the order of 10 µW. However, the emission of the nanowire-based LED shows a spotty and polychromatic emission. By using a confocal microscope, we have been able to improve the spatial resolution of the optical characterizations down to the submicrometre scale that can be assessed to a single nanowire. Detailed µ-electroluminescent characterization (emission wavelength and output power) over a representative number of single nanowires provides new insights into the vertically integrated nanowire-based LED operation. By combining both µ-electroluminescent and µ-photoluminescent excitation, we have experimentally shown that electrical injection failure is the major source of losses in these nanowire-based LEDs.

A single-step electron beam lithography of buried nanostructures using cathodoluminescence imaging and low temperature.

We report a new electron beam lithography process using the cathodoluminescence properties of semiconductors to visualize nanostructures buried underneath the resist and to subsequently write the pattern associated with these nanostructures. This single-step process could be used, for example, to make electrical contacts to nanowires (as illustrated in this work) or to design a photonic crystal resonator centered on a single quantum dot. Fabrication speed and positioning accuracy are significantly increased as compared to the standard process since no alignment marks and the mapping step of the nanostructures with respect to these marks are needed. We show also that low temperature (down to 5 K) could be used to improve the observation of the nanostructures through the resist while keeping very good spatial resolution.

Spatial inhomogeneity of donor bound exciton emission from ZnO nanostructures grown on Si.

We report low temperature cathodoluminescence spectroscopy measurements of the band edge emission from ZnO nanostructures grown by vapour phase transport on Si. A range of donor bound exciton emission lines are found and the Al-related emission at 3.3605 eV in particular shows a marked inhomogeneity in its distribution throughout the sample. Increased 3.3605 eV emission is seen at a range of locations in nanorods and nanosheets where different nanostructures cross or coalesce, suggesting aggregation of Al donors in ZnO in regions of crystal structure disruption. However, localized crystal structure disruption appears to be a necessary rather than a sufficient condition for Al aggregation, since increased 3.3605 eV emission is seen only in such regions, but not all such regions show increased emission, implying that the microscopic nature of such regions is important in determining Al aggregation. Supporting data are presented from well-aligned, non-crossing, nanorods on a-sapphire.

Dynamics of long-range ordering in an exciton-polariton condensate.

We report on time-resolved measurements of the first order spatial coherence in an exciton-polariton Bose-Einstein condensate. Long-range spatial coherence is found to set in right at the onset of stimulated scattering, on a picosecond time scale. The coherence reaches its maximum value after the population and decays slowly, staying up to a few hundred picoseconds. This behavior can be qualitatively reproduced, using a stochastic classical field model describing interaction between the polariton condensate and the exciton reservoir within a disordered potential.

Formation of an exciton polariton condensate: thermodynamic versus kinetic regimes.

We measure the polariton distribution function and the condensation threshold versus the photon-exciton detuning and the lattice temperature in a CdTe microcavity under nonresonant pumping. The results are reproduced by simulations using semiclassical Boltzmann equations. At negative detuning we find a kinetic condensation regime: the distribution is not thermal and the threshold is governed by the relaxation kinetics. At positive detuning, the distribution becomes thermal and the threshold is governed by the thermodynamic parameters of the system. Both regimes are a manifestation of polariton lasing, whereas only the latter is related to Bose-Einstein condensation defined as an equilibrium phase transition.

Intrinsic decoherence mechanisms in the microcavity polariton condensate.

The fundamental mechanisms which control the phase coherence of the polariton Bose-Einstein condensate (BEC) are determined. It is shown that the combination of number fluctuations and interactions leads to decoherence with a characteristic Gaussian decay of the first-order correlation function. This line shape, and the long decay times ( approximately 150 ps) of both first- and second-order correlation functions, are explained quantitatively by a quantum-optical model which takes into account interactions, fluctuations, and gain and loss in the system. Interaction limited coherence times of this type have been predicted for atomic BECs, but are yet to be observed experimentally.

Synchronized and desynchronized phases of exciton-polariton condensates in the presence of disorder.

Condensation of exciton polaritons in semiconductor microcavities takes place despite in-plane disorder. Below the critical density, the inhomogeneity of the disorder limits the spatial extension of the ground state. Above the critical density, in the presence of weak disorder, this limitation is spontaneously overcome by the nonlinear interaction, resulting in an extended synchronized phase. In the case of strong disorder, several non-phase-locked condensates can be evidenced. The transition from a synchronized phase to a desynchronized phase is addressed by sampling the cavity disorder.

Second-order time correlations within a polariton Bose-Einstein condensate in a CdTe microcavity.

Second-order time correlations of polaritons have been measured across the condensation threshold in a CdTe microcavity. The onset of Bose-Einstein condensation is marked by the disappearance of photon bunching, demonstrating the transition from a thermal-like state to a coherent state. Coherence is, however, degraded with increasing polariton density, most probably as a result of self-interaction within the condensate and scatterings with noncondensed excitons and polaritons. Such behavior clearly differentiates polariton Bose condensation from photon lasing.