Recently, metal nanoparticle surface coatings have been found to significantly enhance the ultra-violet luminescence intensity from ZnO, providing a viable means to mitigate optical losses and improve LED performance. Although there is general agreement that resonantly excited Localized Surface Plasmons (LSPs) in metal nanoparticles can directly couple to excitons in the semiconductor increasing their spontaneous emission rate, the exact mechanisms involved in this phenomenon are currently not fully understood. In this work, LSP-exciton coupling in bulk and nanostructured ZnO coated with a 2 nm Al nanoparticle layer is investigated using correlative photoluminescence and depth-resolved cathodoluminescence and time-resolved photoluminescence spectroscopy. Temperature-resolved cathodoluminescence and photoluminescence measurements from 10 K to 250 K show free exciton (FX) emission enhancement factors up to 12x at 80 K, and reveal that the FX couple more efficiently to the LSPs compared to the localized donor-bound excitons. A strong polarization dependence between the LSPs and FX is observed where FX transitions are more strongly enhanced when polarized in the same direction as the electric field of the incident excitation, which is different for laser and electron beam sources. This result indicates that selective enhancement of the excitonic emission peaks in the ZnO coated with Al nanoparticles can be achieved by choosing the appropriate ZnO substrate orientation.
Impurity‐vacancy centers in diamond offer a new class of robust photon sources with versatile quantum properties. While individual color centers commonly act as single‐photon sources, their ensembles have been theoretically predicted to have tunable photon‐emission statistics. Importantly, the particular type of excitation affects the emission properties of a color center ensemble within a diamond crystal. While optical excitation favors non‐synchronized excitation of color centers within an ensemble, electron‐beam excitation can synchronize the emitters excitation and thereby provides a control of the second‐order correlation function g2 (0). In this letter, we demonstrate experimentally that the photon stream from an ensemble of color centers can exhibit g2 (0) both above and below unity, thereby confirming long standing theoretical predictions by Meuret et al. [S. Meuret, L. H. G. Tizei, T. Cazimajou, et al., “Photon bunching in cathodoluminescence,” Phys. Rev. Lett. , vol. 114, no. 19, p. 197401, 2015.]. Such a photon source based on an ensemble of few color centers in a diamond crystal provides a highly tunable platform for informational technologies operating at room temperature.
Large reflection losses at interfaces in light-emitting semiconductor devices cause a significant reduction in their light emission and energy efficiencies. Metal nanoparticle (NP) surface coatings have been demonstrated to increase the light extraction efficiency from planar high refractive index semiconductor surfaces. This emission enhancement in Au NP-coated ZnO is widely attributed to involvement of a green (∼ 2.5 eV) deep level ZnO defect exciting localized surface plasmons in the NPs. In this work, we achieve a 6 times enhancement of the ultra-violet excitonic emission in ZnO nanorods coated with 5 nm Au NPs without the aid of ZnO defects. Cathodoluminescence (CL) and photoluminescence (PL) spectroscopy revealed that the increased UV emission is due to the formation of an additional fast excitonic relaxation pathway. Concurrent CL-PL measurements ruled out the presence of charge transfer mechanism in the emission enhancement process. While time-resolved PL confirmed the existence of a new excitonic recombination channel that is attributed to exciton relaxation via the excitation of rapid non-radiative Au interband transitions that increases the UV spontaneous emission rate. Our results establish that ZnO defect levels ∼ 2.5 eV are not required to facilitate Au NP induced enhancement of the ZnO UV emission.
Cathodoluminescence spectroscopy in conjunction with second-order auto-correlation measurements of allows to extensively study the synchronization of photon emitters in low-dimensional structures. Co-existing excitons in two-dimensional transition metal dichalcogenide monolayers provide a great source of identical photon emitters which can be simultaneously excited by an electron. Here, we demonstrate large photon bunching with up to of a tungsten disulfide monolayer (WS2), exhibiting a strong dependence on the electron-beam current. To further improve the excitation synchronization and the electron-emitter interaction, we show exemplary that the careful selection of a simple and compact geometry—a thin, monocrystalline gold nanodisk—can be used to realize a record-high bunching of up to . This approach to control the electron excitation of excitons in a WS2monolayer allows for the synchronization of photon emitters in an ensemble, which is important to further advance light information and computing technologies.
Microcrystalline Cs2AgxNa1−xBiyIn1−yCl6 perovskites with tailored composition emitting broadband yellow-white photoluminescence with a quantum yield of up to 92% were produced by a new “green” approach under ambient conditions.