Controlling of lattice strains for crack-free and strong ferroelectric barium titanate films by post-thermal treatment.

In this study, we experimentally demonstrate fabrication of ultra-smooth and crystalline barium titanate (BTO) films on magnesium oxide (MgO) substrates by engineering lattice strain and crystal structure via thermal treatment. We observe that oxygen-depleted deposition allows growth of highly strained BTO films on MgO substrates with crack-free surface. In addition, post-thermal treatment relaxes strain, resulting in an enhancement of ferroelectricity. Surface roughening of the BTO films caused by recrystallization during post-thermal treatment is controlled by chemical-mechanical polishing (CMP) to retain their initial ultra-smooth surfaces. From Raman spectroscopy, reciprocal space map (RSM), and capacitance-voltage (C-V) curve measurements, we confirm that the ferroelectricity of BTO films strongly depend on the relaxation of lattice strain and the phase transition from a-axis to c-axis oriented crystal structure.

A Super-Boosted Hybrid Plasmonic Upconversion Process for Photodetection at 1550 nm Wavelength.

A super-boosted hybrid plasmonic upconversion (UC) architecture comprising a hierarchical plasmonic upconversion (HPU) film and a polymeric microlens array (MLA) film is proposed for efficient photodetection at a wavelength of 1550 nm. Plasmonic metasurfaces and Au core-satellite nanoassembly (CSNA) films can strongly induce a more effective plasmonic effect by providing numerous hot spots in an intense local electromagnetic field up to wavelengths exceeding 1550 nm. Hence, significant UC emission enhancement is realized via the amplified plasmonic coupling of an HPU film comprising an Au CSNA and UC nanoparticles. Furthermore, an MLA polymer film is synergistically coupled with the HPU film, thereby focusing the incident near-infrared light in the micrometer region, including the plasmonic nanostructure area. Consequently, the plasmonic effect super-boosted by microfocusing the incident light, significantly lowers the detectable power limit of a device, resulting in superior sensitivity and responsivity at weak excitation powers. Finally, a triple-cation perovskite-based photodetector coupled with the hybrid plasmonic UC film exhibits the excellent values of responsivity and detectivity of 9.80 A W-1 and 8.22 × 1012 Jones at a weak power density of ≈0.03 mW cm-2 , respectively, demonstrating that the device performance is enhanced by more than 104 magnitudes over a reference sample.

Comparative Chemico-Physical Analyses of Strain-Free GaAs/Al0.3Ga0.7As Quantum Dots Grown by Droplet Epitaxy.

We investigate the quantum confinement effects on excitons in several types of strain-free GaAs/Al 0 . 3 Ga 0 . 7 As droplet epitaxy (DE) quantum dots (QDs). By performing comparative analyses of energy-dispersive X-ray spectroscopy with the aid of a three-dimensional (3D) envelope-function model, we elucidate the individual quantum confinement characteristics of the QD band structures with respect to their composition profiles and the asymmetries of their geometrical shapes. By precisely controlling the exciton oscillator strength in strain-free QDs, we envisage the possibility of tailoring light-matter interactions to implement fully integrated quantum photonics based on QD single-photon sources (SPSs).

Highly transparent phototransistor based on quantum-dots and ZnO bilayers for optical logic gate operation in visible-light.

Highly transparent optical logic circuits operated with visible light signals are fabricated using phototransistors with a heterostructure comprised of an oxide semiconductor (ZnO) with a wide bandgap and quantum dots (CdSe/ZnS QDs) with a small bandgap. ZnO serves as a highly transparent active channel, while the QDs absorb visible light and generate photoexcited charge carriers. The induced charge carriers can then be injected into the ZnO conduction band from the QD conduction band, which enables current to flow to activate the phototransistor. The photoexcited charge transfer mechanism is investigated using time-resolved photoluminescence spectroscopy, scanning Kelvin probe microscopy, and ultraviolet photoelectron spectroscopy. Measurements show that carriers in the QD conduction band can transfer to the ZnO conduction band under visible light illumination due to a change in the Fermi energy level. Moreover, the barrier for electron injection into the ZnO conduction band from the QD conduction band is low enough to allow photocurrent generation in the QDs/ZnO phototransistor. Highly transparent NOT, NOR, and NAND optical logic circuits are fabricated using the QDs/ZnO heterostructure and transparent indium tin oxide electrodes. This work provides a means of developing highly transparent optical logic circuits that can operate under illumination with low-energy photons such as those found in visible light.

Strain-induced control of a pillar cavity-GaAs single quantum dot photon source.

Herein, we present the calculated strain-induced control of single GaAs/AlGaAs quantum dots (QDs) integrated into semiconductor micropillar cavities. We show precise energy control of individual single GaAs QD excitons under multi-modal stress fields of tailored micropillar optomechanical resonators. Further, using a three-dimensional envelope-function model, we evaluated the quantum mechanical correction in the QD band structures depending on their geometrical shape asymmetries and, more interestingly, on the practical degree of Al interdiffusion. Our theoretical calculations provide the practical quantum error margins, obtained by evaluating Al-interdiffused QDs that were engineered through a front-edge droplet epitaxy technique, for tuning engineered QD single-photon sources, facilitating a scalable on-chip integration of QD entangled photons.

High-Speed Colloidal Quantum Dot Photodiodes via Accelerating Charge Separation at Metal-Oxide Interface.

With ever-growing technological demands in the imaging sensor industry for autonomous driving and augmented reality, developing sensors that can satisfy not only image resolution but also the response speed becomes more challenging. Herein, the focus is on developing a high-speed photosensor capable of obtaining high-resolution, high-speed imaging with colloidal quantum dots (QDs) as the photosensitive material. In detail, high-speed QD photodiodes are demonstrated with rising and falling times of τr = 28.8 ± 8.34 ns and τf = 40 ± 9.81 ns, respectively, realized by fast separation of electron-hole pairs due to the action of internal electric field at the QD interface, mainly by the interaction between metal oxide and the QD's ligands. Such energy transfer relations are analyzed and interpreted with time-resolved photoluminescence measurements, providing physical understanding of the device and working principles.

Long-distance transmission of broadband near-infrared light guided by a semi-disordered 2D array of metal nanoparticles.

Near-infrared (NIR) waveguides are a key component of planar photonic devices such as optical communication couplers, image sensors, and spectroscopes for chemical or biological molecules. Conventional NIR waveguides used for signal transmission include silicon-on-insulator (SOI) waveguides and channel/ridge-type metal micro-strips. However, these waveguides usually have limitations of either signal delay or signal loss in optically integrated devices. In this study, a novel NIR waveguide composed of a semi-disordered array of metal nanoparticles (sDAMNPs) on Si substrate was proposed, fabricated, and tested. The disordered metallic nanoparticles array is geometrically localized in the form of 1D metal strips, thus replacing sDAMNPs with less lossy micro strip channel waveguides. From the measurements supported by various computational models, the fabricated waveguides operate effectively in the broadband NIR region (1100 to 1700 nm). The waveguide does not support signal transmission in the ultra violet-visible spectrum due to strong signal absorption, scattering, and localization effects inside the metal nanoparticles. Instead, it is capable of transmitting NIR over a distance longer than 100 µm (signal loss ∼3.85 dB per 100 µm for NIR from 1200 to 1600 nm), which is also sufficiently longer than the conventional surface plasmon polariton propagation distance at the metal-Si interface. Compared to a waveguide-free reference, the waveguide exhibited greatly improved signal transmission efficiency up to a factor of 7.42 × 104 at 1367 nm. It also exhibits a high deflection angle sensitivity of 1.89 dB per 0.01 rad, thus efficiently and straightly guiding the broadband NIR signal over a long distance.

Nanocrystalline Titanium Metal-Organic Frameworks for Highly Efficient and Flexible Perovskite Solar Cells.

Flexible perovskite solar cells (PSCs) have attracted considerable attention due to their excellent performance, low-cost, and great potential as an energy supplier for soft electronic devices. In particular, the design of charge transporting layers (CTLs) is crucial to the development of highly efficient and flexible PSCs. Herein, nanocrystalline Ti-based metal-organic framework (nTi-MOF) particles are synthesized to have ca. 6 nm in diameter. These are then well-dispersed in alcohol solvents in order to generate electron transporting layers (ETLs) in PSCs under ambient temperatures using a spin-coating process. The electronic structure of nTi-MOF ETL is found to be suitable for charge injection and transfer from the perovskite to the electrodes. The combination of a [6,6]-phenyl-C61-butyric acid (PCBM) into the nTi-MOF ETL provides for efficient electron transfer and also suppresses direct contact between the perovskite and the electrode. This results in impressive power conversion efficiencies (PCEs) of 18.94% and 17.43% for rigid and flexible devices, respectively. Moreover, outstanding mechanical stability is retained after 700 bending cycles at a bending radius ( r) of 10 mm.

Hole Mobility Characteristics with Surface Roughness on Silicon-on-Insulator Substrate.

Hole mobility characteristics were investigated with surface roughness and silicon-on-insulator (SOI) thickness variations to investigate the influence of surface roughness to mobility. The root mean square roughness varied between 0.16, 0.85 and 10.6 nm in 220, 100 and 40 nm thick SOI samples. Hole mobility was measured and analyzed as a function of effective field and temperature with the variations of surface roughness. The hole mobility, determined by transconductance, greatly decreased with the increase of effective field due to the increased surface roughness scattering in 40 nm thick SOI samples. On the other hand, phonon scattering was a dominant mechanism with the increase of temperature, irrespective of surface roughness and SOI thickness. The induced surface roughness of the devices increases the phonon scattering, thereby reducing the electron and hole mobility. The hole mobility decreases with the roughening of the samples, with the increase of temperature due to increased phonon scattering. Therefore, for enhanced mobility, surface scattering and phonon scattering should be controlled even in atomic scale roughened samples.

Post-thermal-Induced Recrystallization in GaAs/Al0.3Ga0.7As Quantum Dots Grown by Droplet Epitaxy with Near-Unity Stoichiometry.

Here, we investigate the stoichiometry control of GaAs/Al0.3Ga0.7As droplet epitaxy (DE) quantum dots (QDs). Few tens of core nonstoichiometries in the Ga(As) atomic percent are revealed in as-grown "strain-free" QDs using state-of-the-art atomic-scale energy-dispersive X-ray spectroscopy based on transmission electron microscopy. Precise systematic analyses demonstrate a successful quenching of the nonstoichiometry below 2%. The control of the chemical reactions with well-controlled ex situ annealing sheds light on the engineering of a novel single-photon source of strain-free DE QDs free of defects.

A near-infrared photoinverter based on ZnO and quantum-dots.

Near-infrared (NIR) photoswitching transistors have been fabricated using a hybrid structure of zinc oxide (ZnO) and quantum-dots (QDs). The ZnO active layer was prepared using a solution process, while colloidal QDs were inserted between a silicon dioxide (SiO2) gate insulator and a ZnO active layer. The small band gap QDs (1.59 eV) were used to absorb low-energy NIR photons, generate photo-excited carriers, and inject them into the conduction band of the ZnO film. The device with the interfacial QDs induced photocurrents upon exposure to 780 nm-wavelength light. The photoresponsivity of the ZnO/QD device was 0.06 mA W-1, while that of the device without QDs was 1.7 × 10-5 mA W-1, which indicated that the small band gap QDs enabled a photo-induced current when exposed to NIR light. Furthermore, a photoinverter was prepared which was composed of a ZnO/QDs phototransistor and a load resistor. Photoswitching characteristics indicated that the photoinverter was well modulated by a periodic light signal of 780 nm in wavelength. The results demonstrate a useful way to fabricate NIR optoelectronics based on ZnO and QDs.

Solution-processed indium oxide electron transporting layers for high-performance and photo-stable perovskite and organic solar cells.

Interface engineering is considered the key to improving the device performance and stability of solar cells. In particular, TiO2 nanostructures, when used as electron transporting layers (ETLs) in metal halide perovskite solar cells (PSCs), led to excellent power conversion efficiencies (PCEs) of over 20%. They effectively transferred charge carriers from the perovskite and suppressed charge recombination at the interfaces. However, the photocatalytic effect of TiO2 on the perovskite can significantly degrade the device performance under ultraviolet illumination. Therefore, other classes of n-type metal oxides with a wide band gap should be developed to improve their photo-stability. Herein, we demonstrate the development of In2O3 thin films by a solution process and their application as ETLs in PSCs and organic solar cells (OSCs). Pin hole-free In2O3 ETLs obtained by the thermal decomposition of an In precursor thin film exhibit high conductivity (2.49 × 10-4 S cm-1) and low surface roughness (7.33 nm). This leads to impressive PCEs of 14.63% and 3.03% for the PSC and the inverted OSC, respectively. Furthermore, the In2O3-PSC shows better photo-stability than the TiO2-PSC by virtue of the wider band gap of In2O3, which leads to a PCE retention of 74% and 46%, relative to the initial PCE values of the PSC and the inverted OSC, respectively.

Quantum cascade lasers with Y2O3 insulation layer operating at 8.1 µm.

SiO2 is a commonly used insulation layer for QCLs but has high absorption peak around 8 to 10 µm. Instead of SiO2, we used Y2O3 as an insulation layer for DC-QCL and successfully demonstrated lasing operation at the wavelength around 8.1 µm. We also showed 2D numerical analysis on the absorption coefficient of our DC-QCL structure with various parameters such as insulating materials, waveguide width, and mesa angle.

Long-term efficient organic photovoltaics based on quaternary bulk heterojunctions.

A major impediment to the commercialization of organic photovoltaics (OPVs) is attaining long-term morphological stability of the bulk heterojunction (BHJ) layer. To secure the stability while pursuing optimized performance, multi-component BHJ-based OPVs have been strategically explored. Here we demonstrate the use of quaternary BHJs (q-BHJs) composed of two conjugated polymer donors and two fullerene acceptors as a novel platform to produce high-efficiency and long-term durable OPVs. A q-BHJ OPV (q-OPV) with an experimentally optimized composition exhibits an enhanced efficiency and extended operational lifetime than does the binary reference OPV. The q-OPV would retain more than 72% of its initial efficiency (for example, 8.42-6.06%) after a 1-year operation at an elevated temperature of 65 °C. This is superior to those of the state-of-the-art BHJ-based OPVs. We attribute the enhanced stability to the significant suppression of domain growth and phase separation between the components via kinetic trapping effect.

Emissive CdTe/ZnO/GO quasi-core-shell-shell hybrid quantum dots for white light emitting diodes.

Colloidal quantum dots (QDs) have been extensively studied for optoelectronic and biological applications due to their unique physical and optical properties. In particular, among the optoelectronics applications, the white light emitting diode (WLED) has great potential in flat panel displays and solid-state lighting. Herein, we demonstrate a novel, facile, and efficient technique for the synthesis of CdTe/ZnO/GO quasi-core-shell-shell hybrid quantum dots containing the CdTe core with multi shells of ZnO and graphene oxide (GO) and fabrication of WQDLEDs. The CdTe/ZnO/GO quasi-core-shell-shell QDs have a unique strong photoluminescence (PL) peak at 624 nm related to the CdTe core and new weak peaks at 382, 404, 422, and 440 nm due to conjugation with ZnO and GO. Also, in the electroluminescence (EL), multiple emission peaks are observed, which can be correlated to the recombination process inside the CdTe core and also recombination of electrons in the lowest unoccupied molecular orbital (LUMO) and LUMO+2 of GO and holes in the valence band (VB) of ZnO. The QDLEDs show clear white color emission with a maximum luminance value of about 480 cd m-2 with Commission Internationale de l'Eclairage (CIE) color coordinates of (0.35, 0.28).

Alternative Patterning Process for Realization of Large-Area, Full-Color, Active Quantum Dot Display.

Although various colloidal quantum dot (QD) coating and patterning techniques have been developed to meet the demands in optoelectronic applications over the past years, each of the previously demonstrated methods has one or more limitations and trade-offs in forming multicolor, high-resolution, or large-area patterns of QDs. In this study, we present an alternative QD patterning technique using conventional photolithography combined with charge-assisted layer-by-layer (LbL) assembly to solve the trade-offs of the traditional patterning processes. From our demonstrations, we show repeatable QD patterning process that allows multicolor QD patterns in both large-area and microscale. Also, we show that the QD patterns are robust against additional photolithography processes and that the thickness of the QD patterns can be controlled at each position. To validate that this process can be applied to actual device applications as an active material, we have fabricated inverted, differently colored, active QD light-emitting device (QD-LED) on a pixelated substrate, which achieved maximum electroluminescence intensity of 23 770 cd/m2, and discussed the results. From our findings, we believe that our process provides a solution to achieving both high-resolution and large-scale QD pattern applicable to not only display, but also to practical photonic device research and development.

A Plasmonic Platform with Disordered Array of Metal Nanoparticles for Three-Order Enhanced Upconversion Luminescence and Highly Sensitive Near-Infrared Photodetector.

Three-order enhanced upconversion luminescence from upconversion nanoparticles is suggested by way of a promising platform utilizing a disordered array of plasmonic metal nanoparticles. Its application toward highly sensitive NIR photodetectors is discussed.

Vertically aligned nanostructured TiO2 photoelectrodes for high efficiency perovskite solar cells via a block copolymer template approach.

We fabricated perovskite solar cells with enhanced device efficiency based on vertically oriented TiO2 nanostructures using a nanoporous template of block copolymers (BCPs). The dimension and shape controllability of the nanopores of the BCP template allowed for the construction of one-dimensional (1-D) TiO2 nanorods and two-dimensional (2-D) TiO2 nanowalls. The TiO2 nanorod-based perovskite solar cells showed a more efficient charge separation and a lower charge recombination, leading to better performance compared to TiO2 nanowall-based solar cells. The best solar cells employing 1-D TiO2 nanorods showed an efficiency of 15.5% with VOC = 1.02 V, JSC = 20.0 mA cm(-2) and fill factor = 76.1%. Thus, TiO2 nanostructures fabricated from BCP nanotemplates could be applied to the preparation of electron transport layers for improving the efficiency of perovskite solar cells.

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.