Correlations between Cascaded Photons from Spatially Localized Biexcitons in ZnSe.

Radiative cascades emit correlated photon pairs, providing a pathway for the generation of entangled photons. The realization of a radiative cascade with impurity atoms in semiconductors, a leading platform for the generation of quantum light, would therefore provide a new avenue for the development of entangled photon pair sources. Here we demonstrate a radiative cascade from the decay of a biexciton at an impurity-atom complex in a ZnSe quantum well. The emitted photons show clear temporal correlations revealing the time-ordering of the cascade. Our result establishes impurity atoms in ZnSe as a potential platform for photonic quantum technologies using radiative cascades.

Optical pumping of a single electron spin bound to a fluorine donor in a ZnSe nanostructure.

Here we demonstrate optical pumping of a single electron within a semiconductor nanostructure comprised of a single fluorine donor located within a ZnSe/ZnMgSe quantum well. Experiments were performed to detect optical pumping behavior by observing single photons emitted from the nanostructure when the electron changes spin state. These results demonstrate initialization and read-out of the electron spin qubit and open the door for coherent optical manipulation of a spin by taking advantage of an unconventional nanostructure.

Growth and Electrical Characterization of Hybrid Core/Shell InAs/CdSe Nanowires.

Core-only InAs nanowires (NWs) remain of continuing interest for application in modern optical and electrical devices. In this paper, we utilize the II-VI semiconductor CdSe as a shell for III-V InAs NWs to protect the electron transport channel in the InAs core from surface effects. This unique material configuration offers both a small lattice mismatch between InAs and CdSe and a pronounced electronic confinement in the core with type-I band alignment at the interface between both materials. Under optimized growth conditions, a smooth interface between the core and shell is obtained. Atom probe tomography (APT) measurements confirm substantial diffusion of In into the shell, forming a remote n-type doping of CdSe. Moreover, field-effect transistors (FETs) are fabricated, and the electron transport characteristics in these devices is investigated. Finally, band structure simulations are performed and confirm the presence of an electron transport channel in the InAs core that, at higher gate voltages, extends into the CdSe shell region. These results provide a promising basis toward the application of hybrid III-V/II-VI core/shell nanowires in modern electronics.

Entangling single photons from independently tuned semiconductor nanoemitters.

Quantum communication systems based on nanoscale semiconductor devices is challenged by inhomogeneities from device to device. We address this challenge using ZnMgSe/ZnSe quantum-well nanostructures with local laser-based heating to tune the emission of single impurity-bound exciton emitters in two separate devices. The matched emission in combination with photon bunching enables quantum interference from the devices and allows the postselection of polarization-entangled single photons. The ability to entangle single photons emitted from nanometer-sized sources separated by macroscopic distances provides an essential step for a solid-state realization of a large-scale quantum optical network. This paves the way toward measurement-based entanglement generation between remote electron spins localized at macroscopically separated fluorine impurities.

Efficient Single-Photon Sources Based on Chlorine-Doped ZnSe Nanopillars with Growth Controlled Emission Energy.

Isolated impurity states in epitaxially grown semiconductor systems possess important radiative features such as distinct wavelength emission with a very short radiative lifetime and low inhomogeneous broadening, which make them promising for the generation of indistinguishable single photons. In this study, we investigate chlorine-doped ZnSe/ZnMgSe quantum well (QW) nanopillar (NP) structures as a highly efficient solid-state single-photon source operating at cryogenic temperatures. We show that single photons are generated due to the radiative recombination of excitons bound to neutral Cl atoms in ZnSe QW and the energy of the emitted photon can be tuned from about 2.85 down to 2.82 eV with ZnSe well width increase from 2.7 to 4.7 nm. Following the developed advanced technology, we fabricate NPs with a diameter of about 250 nm using a combination of dry and wet-chemical etching of epitaxially grown ZnSe/ZnMgSe QW structures. The remaining resist mask serves as a spherical- or cylindrical-shaped solid immersion lens on top of NPs and leads to the emission intensity enhancement by up to an order of magnitude in comparison to the pillars without any lenses. NPs with spherical-shaped lenses show the highest emission intensity values. The clear photon-antibunching effect is confirmed by the measured value of the second-order correlation function at a zero time delay of 0.14. The developed single-photon sources are suitable for integration into scalable photonic circuits.

Mechanism of the living lactide polymerization mediated by robust zinc guanidine complexes.

Zinc bis(chelate) guanidine complexes promote living lactide polymerization at elevated temperatures. By means of kinetic and spectroscopic analyses the mechanism has been elucidated for these special initiators that make use of neutral N-donor ligands. The neutral guanidine function initiates the polymerization by a nucleophilic ring-opening attack on the lactide molecule. DFT calculations on the first ring-opening step show that the guanidine is able to act as a nucleophile. Three transition states were located for ligand rearrangement, nucleophilic attack, and ring-opening. The second ring-opening step was modeled as a representation for the chain growth because here, the lactate alcoholate opens the second lactide molecule via two transition states (nucleophilic attack and ring-opening). Additionally, the resulting reaction profile proceeds overall exothermically, which is the driving force for the reaction. The experimental and calculated data are in good agreement and the presented mechanism explains why the polymerization proceeds without co-initiators.

Strain Compensation in Single ZnSe/CdSe Quantum Wells: Analytical Model and Experimental Evidence.

The lattice mismatch between CdSe and ZnSe is known to limit the thickness of ZnSe/CdSe quantum wells on GaAs (001) substrates to about 2-3 monolayers. We demonstrate that this thickness can be enhanced significantly by using In0.12Ga0.88As pseudo substrates, which generate alternating tensile and compressive strains in the ZnSe/CdSe/ZnSe layers resulting in an efficient strain compensation. This method enables to design CdSe/ZnSe quantum wells with CdSe thicknesses ranging from 1 to 6 monolayers, covering the whole visible spectrum. The strain compensation effect is investigated by high resolution transmission electron microscopy and supported by molecular statics simulations. The model approach with the supporting experimental measurements is sufficiently general to be also applied to other highly mismatched material combinations for the design of advanced strained heterostructures.

Indistinguishable photons from independent semiconductor nanostructures.

We demonstrate quantum interference between photons generated by the radiative decay processes of excitons that are bound to isolated fluorine donor impurities in ZnSe/ZnMgSe quantum-well nanostructures. The ability to generate single photons from these devices is confirmed by autocorrelation experiments, and the indistinguishability of photons emitted from two independent nanostructures is confirmed via a Hong-Ou-Mandel dip. These results indicate that donor impurities in appropriately engineered semiconductor structures can portray atomlike homogeneity and coherence properties, potentially enabling scalable technologies for future large-scale optical quantum computers and quantum communication networks.