Brightness and purity of a room-temperature single-photon source in the blue-green range.

We discuss a promising solid-state system that emits single photons at room temperature in the blue-green range, making it an attractive candidate for quantum communications in free space and underwater. The active element is a core-shell ZnSe tapered nanowire embedding a single CdSe quantum dot grown by molecular beam epitaxy. A patterned substrate enables a comprehensive study of a single nanowire using various methods. Our source shows potential for achieving a total brightness of 0.17 photon per pulse and anti-bunching with g(2)(0) < 0.3 within a restricted spectral window. Additionally, we analyze the impact of charged excitons on the g(2)(0) value in different spectral ranges.

Controlled Coherent Coupling in a Quantum Dot Molecule Revealed by Ultrafast Four-Wave Mixing Spectroscopy.

Semiconductor quantum dot molecules are considered promising candidates for quantum technological applications due to their wide tunability of optical properties and coverage of different energy scales associated with charge and spin physics. While previous works have studied the tunnel-coupling of the different excitonic charge complexes shared by the two quantum dots by conventional optical spectroscopy, we here report on the first demonstration of a coherently controlled interdot tunnel-coupling focusing on the quantum coherence of the optically active trion transitions. We employ ultrafast four-wave mixing spectroscopy to resonantly generate a quantum coherence in one trion complex, transfer it to and probe it in another trion configuration. With the help of theoretical modeling on different levels of complexity, we give an instructive explanation of the underlying coupling mechanism and dynamical processes.

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.

Operation of a fiber-coupled laser-cooler down to cryogenic temperatures.

We report on the optical cooling of a 7.5%Yb:LiYF4 crystal down to 125 K in a multi-pass Herriott absorption cell, coupled via a single mode polarization maintaining optical fiber to the laser source. This configuration, never exploited before, is more practical for potential applications, in particular for spaceborne cryogenics setups. Moreover, the temperature reached is exactly the one needed in many setup embarked in small and medium satellites. We evaluate the heat load on the crystal at the minimum attainable temperature, which is comparable to state of the art systems.

Operation of a fiber-coupled laser-cooler down to cryogenic temperatures: publisher's note.

This publisher's note contains a correction to [Opt. Express30, 12929 (2022)10.1364/OE.448930].

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.

Aqueous Synthesis of DNA-Functionalized Near-Infrared AgInS2/ZnS Core/Shell Quantum Dots.

Biocompatibility, biofunctionality, and chemical stability are essential criteria to be fulfilled by quantum dot (QD) emitters for bio-imaging and -sensing applications. In addition to these criteria, achieving efficient near-infrared (NIR) emission with nontoxic QDs remains very challenging. In this perspective, we developed water-soluble NIR-emitting AgInS2/ZnS core/shell (AIS/ZnS) QDs functionalized with DNA. The newly established aqueous route relying on a two-step hot-injection synthesis led to highly luminescent chalcopyrite-type AIS/ZnS core/shell QDs with an unprecedented photoluminescence quantum yield (PLQY) of 55% at 700 nm and a long photoluminescence (PL) decay time of 900 ns. Fast and slow hot injection of the precursors were compared for the AIS core QD synthesis, yielding a completely different behavior in terms of size, size distribution, stoichiometry, and crystal structure. The PL peak positions of both types of core QDs were 710 (fast) and 760 nm (slow injection) with PLQYs of 36 and 8%, respectively. The slow and successive incorporation of the Zn and S precursors during the subsequent shell growth step on the stronger emitting cores promoted the formation of a three-monolayer thick ZnS shell, evidenced by the increase of the average QD size from 3.0 to 4.8 nm. Bioconjugation of the AIS/ZnS QDs with hexylthiol-modified DNA was achieved during the ZnS shell growth, resulting in a grafting level of 5-6 DNA single strands per QD. The successful chemical conjugation of DNA was attested by UV-vis spectroscopy and agarose gel electrophoresis. Importantly, surface plasmon resonance imaging experiments using complementary DNA strands further corroborated the successful coupling and the stability of the AIS/ZnS-DNA QD conjugates as well as the preservation of the biological activity of the anchored DNA. The strong NIR emission and biocompatibility of these AIS/ZnS-DNA QDs provide a high potential for their use in biomedical applications.

Coherence and Density Dynamics of Excitons in a Single-Layer MoS2 Reaching the Homogeneous Limit.

We measure the coherent nonlinear response of excitons in a single layer of molybdenum disulfide embedded in hexagonal boron nitride, forming a h-BN/MoS2/ h-BN heterostructure. Using four-wave mixing microscopy and imaging, we correlate the exciton inhomogeneous broadening with the homogeneous one and population lifetime. We find that the exciton dynamics is governed by microscopic disorder on top of the ideal crystal properties. Analyzing the exciton ultrafast density dynamics using amplitude and phase of the response, we investigate the relaxation pathways of the resonantly driven exciton population. The surface protection via encapsulation provides stable monolayer samples with low disorder, avoiding surface contaminations and the resulting exciton broadening and modifications of the dynamics. We identify areas localized to a few microns where the optical response is totally dominated by homogeneous broadening. Across the sample of tens of micrometers, weak inhomogeneous broadening and strain effects are observed, attributed to the remaining interaction with the h-BN and imperfections in the encapsulation process.

Emergence of quantum correlations from interacting fibre-cavity polaritons.

Over the past decade, exciton-polaritons in semiconductor microcavities have revealed themselves as one of the richest realizations of a light-based quantum fluid1, subject to fascinating new physics and potential applications2-6. For instance, in the regime of large two-body interactions, polaritons can be used to manipulate the quantum properties of a light field7-9. In this work, we report on the emergence of quantum correlations in laser light transmitted through a fibre-cavity polariton system. We observe a dispersive shape of the autocorrelation function around the polariton resonance that indicates the onset of this regime. The weak amplitude of these correlations indicates a state that still remains far from a low-photon-number state. Nonetheless, given the underlying physical mechanism7, our work opens up the prospect of eventually using polaritons to turn laser light into single photons.

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.

Cathodoluminescence spectroscopy of plasmonic patch antennas: towards lower order and higher energies.

We report on the cathodoluminescence characterization of Au, Al and a Au/Al bimetal circular plasmonic patch antennas, with disk diameter ranging from 150 to 900 nm. It allows us access to monomode operation of the antennas down to the fundamental dipolar mode, in contrast to previous studies on similar systems. Moreover we show that we can shift the operation range of the antennas towards the blue spectral range by using Al. Our experimental results are compared to a semi-analytical model that provides qualitative insight on the mode structure sustained by the antennas.

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.

Deterministic radiative coupling between plasmonic nanoantennas and semiconducting nanowire quantum dots.

We report on the deterministic coupling between single semiconducting nanowire quantum dots emitting in visible and plasmonic Au nanoantennas. Both systems are separately and carefully characterized through micro-photoluminescence and cathodoluminescence. A two-step realignment process using cathodoluminescence allows for electron-beam lithography of Au antennas near individual nanowire quantum dots with a precision of 50 nm. A complete set of optical properties was measured before and after antenna fabrication. They evidence both an increase of the nanowire absorption, and an improvement of the quantum dot emission rate up to a factor of two in presence of the antenna.

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.