Ultrafast and Bright Quantum Emitters from the Cavity-Coupled Single Perovskite Nanocrystals.

Perovskite nanocrystals (NCs) have attracted increasing interest in the realization of single-photon emitters owing to their ease of chemical synthesis, wide spectral tunability, fast recombination rate constant, scalability, and high quantum yield. However, the integration of a single perovskite NC into a photonic structure has yet to be accomplished. In this work, the integration of a highly stable individual zwitterionic ligand-based CsPbBr3 perovskite NC with a circular Bragg grating (CBG) is successfully demonstrated. The far-field radiation pattern of the NC inside the CBG exhibits high directionality toward a low azimuthal angle, which is consistent with the simulation results. A 5.4-fold enhancement in brightness is observed due to an increase in collection efficiency. Moreover, a 1.95-fold increase in the recombination rate constant is achieved. This study offers ultrafast (<100 ps) single-photon emission and an improved brightness of perovskite NCs, which are critical factors for practical quantum optical applications.

Single Quantum Dot Selection and Tailor-Made Photonic Device Integration using a Nanoscale-Focus Pinspot.

Among the diverse platforms of quantum light sources, epitaxially grown semiconductor quantum dots (QDs) are one of the most attractive workhorses for realizing quantum photonic technologies owing to their outstanding brightness and scalability. However, the spatial and spectral randomness of most QDs severely hinders the construction of large-scale photonic platforms. In this work, a methodology is presented to deterministically integrate single QDs with tailor-made photonic structures. A nondestructive luminescence picking method termed as nanoscale-focus pinspot (NFP) is applied using helium-ion microscopy to reduce the luminous QD density while retaining the surrounding medium. A single QD emission is only extracted out of the high-density ensemble QDs. Then the tailor-made photonic structure of a circular Bragg reflector (CBR) is designed and deterministically integrated with the selected QD. Given that the microscopy can image with nanoscale resolution and apply NFP in situ, photonic devices can be deterministically fabricated on target QDs. The extraction efficiency of the NFP-selected QD emission is improved by 25 times after the CBR integration. Since the NFP method only controls the luminescence without destroying the medium, it is applicable to various photonic structures such as photonic waveguides or photonic crystal cavities regardless of materials.

Electrically Driven Sub-Micrometer Light-Emitting Diode Arrays Using Maskless and Etching-Free Pixelation.

For decades, group-III-nitride-based light-emitting diodes (LEDs) have been regarded as a light emitting source for future displays by virtue of their novel properties such as high efficiency, brightness, and stability. Nevertheless, realization of high pixel density displays is still challenging due to limitations of pixelation methods. Here, a maskless and etching-free micro-LED (µLED) pixelation method is developed via tailored He focused ion beam (FIB) irradiation technique, and electrically driven sub-micrometer-scale µLED pixel arrays are demonstrated. It is confirmed that optical quenching and electrical isolation effects are simultaneously induced at a certain ion dose (≈1014 ions cm-2 ) without surface damage. Furthermore, highly efficient µLED pixel arrays at sub-micrometer scale (square pixel, 0.5 µm side length) are fabricated. Their pixelation and brightness are verified by various optical measurements such as cathodo-, photo-, and electroluminescence. It is expected that the FIB-induced optical quenching and electrical isolation method can pioneer a new defect engineering technology not only for µLED fabrication, but also for sub-micrometer-scale optoelectronic devices.

Enhancement of Single-Photon Purity and Coherence of III-Nitride Quantum Dot with Polarization-Controlled Quasi-Resonant Excitation.

III-Nitride semiconductor-based quantum dots (QDs) play an essential role in solid-state quantum light sources because of their potential for room-temperature operation. However, undesired background emission from the surroundings deteriorates single-photon purity. Moreover, spectral diffusion causes inhomogeneous broadening and limits the applications of QDs in quantum photonic technologies. To overcome these obstacles, it is demonstrated that directly pumping carriers to the excited state of the QD reduces the number of carriers generated in the vicinities. The polarization-controlled quasi-resonant excitation is applied to InGaN QDs embedded in GaN nanowire. To analyze the different excitation mechanisms, polarization-resolved absorptions are investigated under the above-barrier bandgap, below-barrier bandgap, and quasi-resonant excitation conditions. By employing polarization-controlled quasi-resonant excitation, the linewidth is reduced from 353 to 272 µeV, and the second-order correlation value is improved from 0.470 to 0.231. Therefore, a greater single-photon purity can be obtained at higher temperatures due to decreased linewidth and background emission.

Highly Efficient Vacuum-Evaporated CsPbBr3 Perovskite Light-Emitting Diodes with an Electrical Conductivity Enhanced Polymer-Assisted Passivation Layer.

Highly efficient vacuum-deposited CsPbBr3 perovskite light-emitting diodes (PeLEDs) are demonstrated by introducing a separate polyethylene oxide (PEO) passivation layer. A CsPbBr3 film deposited on the PEO layer via thermal co-evaporation of CsBr and PbBr2 exhibits an almost 50-fold increase in photoluminescence quantum yield intensity compared to a reference sample without PEO. This enhancement is attributed to the passivation of interfacial defects of the perovskite, as evidenced by temperature-dependent photoluminescence measurements. However, direct application of PEO to an LED device is challenging because of the electrically insulating nature of PEO. This issue is solved by doping PEO layers with MgCl2. This strategy results in an enhanced luminance and external quantum efficiency (EQE) of up to 6887 cd m-2 and 7.6%, respectively. To the best of our knowledge, this is the highest EQE reported to date among vacuum-deposited PeLEDs.

Nanoscale Focus Pinspot for High-Purity Quantum Emitters via Focused-Ion-Beam-Induced Luminescence Quenching.

Epitaxially grown quantum dots (QDs), especially embedded in photonic structures, play an essential role in various quantum photonic systems as on-demand single-photon sources. However, these QDs often suffer from adjacent unwanted emitters, which contribute to the background noise of the QD emission and fundamentally limit the single-photon purity. In this paper, a nanoscale focus pinspot (NFP) technique using focused-ion-beam-induced luminescence quenching enables us to improve single-photon purity from site-controlled QD as a proof-of-concept experiment. The optical quality of the QD emission is not degraded while the signal-to-noise ratio of the QD is improved. Moreover, the QD after the NFP technique reveals the single-photon nature at further elevated temperatures owing to the reduced background noise. As the NFP technique is nondestructive, it retains the apparent physical structures and photonic functions, thereby indicating its promising potential for applying diverse high-purity quantum emitters, particularly integrated in photonic devices and circuits.