Modeling the co-assembly of binary nanoparticles.

In this work, we present a binary assembly model that can predict the co-assembly structure and spatial frequency spectra of monodispersed nanoparticles with two different particle sizes. The approach relies on an iterative algorithm based on geometric constraints, which can simulate the assembly patterns of particles with two distinct diameters, size distributions, and at various mixture ratios on a planar surface. The two-dimensional spatial-frequency spectra of the modeled assembles can be analyzed using fast Fourier transform analysis to examine their frequency content. The simulated co-assembly structures and spectra are compared with assembled nanoparticles fabricated using transfer coating method are in qualitative agreement with the experimental results. The co-assembly model can also be used to predict the peak spatial frequency and the full-width at half-maximum bandwidth, which can lead to the design of the structure spectra by selection of different monodispersed particles. This work can find applications in fabrication of non-periodic nanostructures for functional surfaces, light extraction structures, and broadband nanophotonics.

Recovering cavity effects in corrugated organic light emitting diodes.

Cavity effects play an important role in determining the out-coupling efficiency of an OLED. By fabricating OLEDs on corrugated substrates, the waveguide and SPP modes can be extracted by diffraction. However, corrugation does not always lead to an enhancement in out-coupling efficiency due to the reduction of the electrode reflectance and hence the cavity effects. Based on the results of our rigorous couple-wave analysis (RCWA) simulation, we found that the cavity effects can be partially recovered using a low index Teflon layer inserted between the ITO anode and the substrate due to the enhancement of the reflectance of the corrugated electrodes. To verify the simulation results, we fabricated corrugated OLEDs having a low-index Teflon interlayer with an EQE of 36%, which is 29% higher than an optimized planar OLED. By experimentally measuring the OLED air mode dispersion, we confirm the cavity emission of a corrugated OLED is enhanced by the low index layer.

Perovskite Solar Cells on Corrugated Substrates with Enhanced Efficiency.

Organometallic halide perovskites solar cells are fabricated on nano-scaled corrugated substrates using a sequential deposition method. The corrugated substrates are fabricated using colloidal lithography followed by reactive ion etching. The corrugated structure is found to accelerate the chemical reaction between the sequentially deposited lead iodide (PbI2 ) and methyl ammonium iodide layers to form stoichiometric perovskite films, and the corrugated morphology is preserved at the interface of the hole transport layer (HTL) and the perovskite layer. The shunt resistance of the corrugated devices is found to be higher than that of the planar devices, leading to a higher open circuit voltage (VOC ) and fill factor (FF) in the corrugated devices. Finite-difference time-domain simulation is carried out on both planar and corrugated devices. The results revealed that light absorption is enhanced in the corrugated devices due to the corrugated HTL/perovskite interface, resulting in a significantly higher short circuit current (JSC ) observed in the corrugated devices. As a result, the average power conversion efficiency increases from 8.7% for the planar devices to 13% for the corrugated devices.

Inorganic UV-Visible-SWIR Broadband Photodetector Based on Monodisperse PbS Nanocrystals.

Solution-processed inorganic UV-visible short-wave-infrared photodetectors with light sensitivity from 350 nm to 2000 nm are fabricated using highly monodispersed large PbS NCs. These devices showed detectivity values over 1 × 10(11) Jones from 350 nm to 2000 nm, and a maximum detectivity value of 1.2 × 10(12) Jones at 1800 nm.

Origin of Sub-Bandgap Electroluminescence in Organic Light-Emitting Diodes.

Sub-bandgap electroluminescence in organic light emitting diodes is a phenomenon in which the electroluminescence turn-on voltage is lower than the bandgap voltage of the emitter. Based on the results of transient electroluminescence (EL) and photoluminescence and electroabsorption spectroscopy measurements, it is concluded that in rubrene/C60 devices, charge transfer excitons are generated at the rubrene/C60 interface under sub-bandgap driving conditions, leading to the formation of triplet excitons, and sub-bandgap EL is the result of the subsequent triplet-triplet annihilation process.

All solution-processed inorganic/organic hybrid permeable metal-base transistor.

All solution-processed inorganic/organic hybrid permeable-base transistor (PMBT) based on nickel oxide emitter and P3HT collector is developed. Due to the high charge injection properties of nickel oxide and spontaneously formed nano-pinholes in the base electrode, the devices exhibit high common-base and common-emitter current gains up to 0.98 and 304, respectively with saturated output current.

Metal-Halide Perovskite Lasers: Cavity Formation and Emission Characteristics.

Hybrid metal-halide perovskites (MHPs) have shown remarkable optoelectronic properties as well as facile and cost-effective processability. With the success of MHP solar cells and light-emitting diodes, MHPs have also exhibited great potential as gain media for on-chip lasers. However, to date, stable operation of optically pumped MHP lasers and electrically driven MHP lasers-an essential requirement for MHP laser's insertion into chip-scale photonic integrated circuits-is not yet demonstrated. The main obstacles include the instability of MHPs in the atmosphere, rudimentary MHP laser cavity patterning methods, and insufficient understanding of emission mechanisms in MHP materials and cavities. This review aims to provide a detailed overview of different strategies to improve the intrinsic properties of MHPs in the atmosphere and to establish an optimal MHP cavity patterning method. In addition, this review discusses different emission mechanisms in MHP materials and cavities and how to distinguish them.

Synthetic principles directing charge transport in low-band-gap dithienosilole-benzothiadiazole copolymers.

Given the fundamental differences in carrier generation and device operation in organic thin-film transistors (OTFTs) and organic photovoltaic (OPV) devices, the material design principles to apply may be expected to differ. In this respect, designing organic semiconductors that perform effectively in multiple device configurations remains a challenge. Following "donor-acceptor" principles, we designed and synthesized an analogous series of solution-processable π-conjugated polymers that combine the electron-rich dithienosilole (DTS) moiety, unsubstituted thiophene spacers, and the electron-deficient core 2,1,3-benzothiadiazole (BTD). Insights into backbone geometry and wave function delocalization as a function of molecular structure are provided by density functional theory (DFT) calculations at the B3LYP/6-31G(d,p) level. Using a combination of X-ray techniques (2D-WAXS and XRD) supported by solid-state NMR (SS-NMR) and atomic force microscopy (AFM), we demonstrate fundamental correlations between the polymer repeat-unit structure, molecular weight distribution, nature of the solubilizing side-chains appended to the backbones, and extent of structural order attainable in p-channel OTFTs. In particular, it is shown that the degree of microstructural order achievable in the self-assembled organic semiconductors increases largely with (i) increasing molecular weight and (ii) appropriate solubilizing-group substitution. The corresponding field-effect hole mobilities are enhanced by several orders of magnitude, reaching up to 0.1 cm(2) V(-1) s(-1) with the highest molecular weight fraction of the branched alkyl-substituted polymer derivative in this series. This trend is reflected in conventional bulk-heterojunction OPV devices using PC(71)BM, whereby the active layers exhibit space-charge-limited (SCL) hole mobilities approaching 10(-3) cm(2) V(-1) s(-1), and yield improved power conversion efficiencies on the order of 4.6% under AM1.5G solar illumination. Beyond structure-performance correlations, we observe a large dependence of the ionization potentials of the polymers estimated by electrochemical methods on polymer packing, and expect that these empirical results may have important consequences on future material study and device applications.

PbSe nanocrystal-based infrared-to-visible up-conversion device.

Low-cost hybrid up-conversion devices with infrared sensitivity to 1.5 µm were obtained by integrating a colloidal PbSe nanocrystal near-infrared sensitizing layer on a green phosphorescent organic light emitting diode. A ZnO nanocrystal hole blocking layer is incorporated in the devices for keeping the device off in the absence of IR excitation. The maximum photon (1.3 µm)-to-photon (0.52 µm) conversion efficiency is 1.3%. The extension (until 1.5 µm) of the near-infrared wavelengths, which can be converted to visible light, may be able to improve night vision.

Curved Mirror Arrays for Light Extraction in Top-Emitting Organic Light-Emitting Diodes.

The light outcoupling efficiency of a top-emitting organic light-emitting diode (OLED) is only about 20%, and the majority of the light is trapped in the waveguide modes and surface plasmon polariton (SPP) modes. Extracting the trapped modes can reduce the device power consumption and improve the operating lifetime. In this study, we demonstrate a top-emitting OLED structure with a dielectric spacer to suppress the SPP mode and with a patterned back mirror to extract the waveguide modes. We examine and compare several curved mirror arrays and conclude that a micromirror array (µMA) can efficiently extract the waveguide modes while minimizing the absorption loss. The optimized µMA device with a semi-transparent top electrode shows a 36% external quantum efficiency, 2 times higher than the referenced device. This optical design can be easily incorporated into a top-emitting device and has a great potential for displays and lighting applications.

Importance of Electric-Field-Independent Mobilities in Thick-Film Organic Solar Cells.

In organic solar cells (OSCs), a thick active layer usually yields a higher photocurrent with broader optical absorption than a thin active layer. In fact, a ∼300 nm thick active layer is more compatible with large-area processing methods and theoretically should be a better spot for efficiency optimization. However, the bottleneck of developing high-efficiency thick-film OSCs is the loss in fill factor (FF). The origin of the FF loss is not clearly understood, and there a direct method to identify photoactive materials for high-efficiency thick-film OSCs is lacking. Here, we demonstrate that the mobility field-dependent coefficient is an important parameter directly determining the FF loss in thick-film OSCs. Simulation results based on the drift-diffusion model reveal that a mobility field-dependent coefficient smaller than 10-3 (V/cm)-1/2 is required to maintain a good FF in thick-film devices. To confirm our simulation results, we studied the performance of two ternary bulk heterojunction (BHJ) blends, PTQ10:N3:PC71BM and PM6:N3:PC71BM. We found that the PTQ10 blend film has weaker field-dependent mobilities, giving rise to a more balanced electron-hole transport at low fields. While both the PM6 blend and PTQ10 blend yield good performance in thin-film devices (∼100 nm), only the PTQ10 blend can retain a FF = 74% with an active layer thickness of up to 300 nm. Combining the benefits of a higher JSC in thick-film devices, we achieved a PCE of 16.8% in a 300 nm thick PTQ10:N3:PC71BM OSC. Such a high FF in the thick-film PTQ10 blend is also consistent with the observation of lower charge recombination from light-intensity-dependent measurements and lower energetic disorder observed in photothermal deflection spectroscopy.

Dithienogermole as a fused electron donor in bulk heterojunction solar cells.

We report the synthesis and bulk heterojunction photovoltaic performance of the first dithienogermole (DTG)-containing conjugated polymer. Stille polycondensation of a distannyl-DTG derivative with 1,3-dibromo-N-octyl-thienopyrrolodione (TPD) results in an alternating copolymer which displays light absorption extending to 735 nm, and a higher HOMO level than the analogous copolymer containing the commonly utilized dithienosilole (DTS) heterocycle. When polyDTG-TPD:PC(70)BM blends are utilized in inverted bulk heterojunction solar cells, the cells display average power conversion efficiencies of 7.3%, compared to 6.6% for the DTS-containing cells prepared in parallel under identical conditions. The performance enhancement is a result of a higher short-circuit current and fill factor in the DTG-containing cells, which comes at the cost of a slightly lower open circuit voltage than for the DTS-based cells.

Directional Polarized Light Emission from Thin-Film Light-Emitting Diodes.

Light-emitting diodes (LEDs) with directional and polarized light emission have many photonic applications, and beam shaping of these devices is fundamentally challenging because they are Lambertian light sources. In this work, using organic and perovskite LEDs (PeLEDs) for demonstrations, by selectively diffracting the transverse electric (TE) waveguide mode while suppressing other optical modes in a nanostructured LED, the authors first demonstrate highly directional light emission from a full-area organic LED with a small divergence angle less than 3° and a TE to transverse magnetic (TM) polarization extinction ratio of 13. The highly selective diffraction of only the TE waveguide mode is possible due to the planarization of the device stack by thermal evaporation and solution processing. Using this strategy, directional and polarized emission from a perovskite LED having a current efficiency 2.6 times compared to the reference planar device is further demonstrated. This large enhancement in efficiency in the PeLED is attributed to a larger contribution from the TE waveguide mode resulting from the high refractive index in perovskite materials.

Direct Acoustic Imaging Using a Piezoelectric Organic Light-Emitting Diode.

Conventional ultrasonic imaging requires acoustic scanning over a target object using a piezoelectric transducer array, followed by signal processing to reconstruct the image. Here, we report a novel ultrasonic imaging device that can optically display an acoustic signal on the surface of a piezoelectric transducer. By fabricating an organic light-emitting diode (OLED) on top of a piezoelectric crystal, lead zirconate titanate (PZT), an acousto-optical piezoelectric OLED (p-OLED) transducer is realized, converting an acoustic wave profile directly to an optical image. Because of the integrated device architecture, the resulting p-OLED features a high acousto-optic conversion efficiency at the resonance frequency, providing a piezoelectric field to drive the OLED. By incorporating an electrode array in the p-OLED, we demonstrate a novel tomographic ultrasound imaging device that is operated without a need for conventional signal processing.

Multi-mode Organic Light-Emitting Diode to Suppress the Viewing Angle Dependence.

A typical top-emitting organic light-emitting diode (OLED) has a strong microcavity effect because of the two reflective electrodes. The cavity effect causes a serious color shift with the viewing angles and restricts the organic layer thickness. To overcome these drawbacks, we design a multi-mode OLED structure with dual-dielectric spacer layers, which extend the cavity length by more than 10 times. This design completely eliminates the intrinsic cavity effect caused by the top and bottom boundaries and provides freedom for the organic layer thickness. We demonstrate these effects in a white multi-mode OLED using a white emitter, which shows a negligible angular chromaticity shift of Δuv = 0.006 from 0 to 70° and a Lambertian emission profile. The simple design and the perfect angular color profiles make the multi-mode OLED structure promising in large-area displays and solid-state lighting applications.

Understanding the Role of Ion Migration in the Operation of Perovskite Light-Emitting Diodes by Transient Measurements.

Perovskite light-emitting diodes have been gaining attention in recent years due to their high efficiencies. Despite of the recent progress made in device efficiency, the operation mechanisms of these devices are still not well understood, especially the effects of ion migration. In this work, the role of ion migration is investigated by measuring the transient electroluminescence and current responses, with both the current and efficiency showing a slow response in a time scale of tens of milliseconds. The results of the charge injection dynamics show that the slow response of the current is attributed to the migration and accumulation of halide ions at the anode interface, facilitating hole injection and leading to a strong charge imbalance. Further, the results of the charge recombination dynamics show that the slow response of the efficiency is attributed to enhanced charge injection facilitated by ion migration, which leads to an increased carrier density favoring bimolecular radiative recombination. Through a combined analysis of both charge injection and recombination dynamics, we finally present a comprehensive picture of the role of ion migration in device operation.

Efficient Energy Funneling in Quasi-2D Perovskites: From Light Emission to Lasing.

Quasi-2D Ruddlesden-Popper halide perovskites with a large exciton binding energy, self-assembled quantum wells, and high quantum yield draw attention for optoelectronic device applications. Thin films of these quasi-2D perovskites consist of a mixture of domains having different dimensionality, allowing energy funneling from lower-dimensional nanosheets (high-bandgap domains) to 3D nanocrystals (low-bandgap domains). High-quality quasi-2D perovskite (PEA)2 (FA)3 Pb4 Br13 films are fabricated by solution engineering. Grazing-incidence wide-angle X-ray scattering measurements are conducted to study the crystal orientation, and transient absorption spectroscopy measurements are conducted to study the charge-carrier dynamics. These data show that highly oriented 2D crystal films have a faster energy transfer from the high-bandgap domains to the low-bandgap domains (<0.5 ps) compared to the randomly oriented films. High-performance light-emitting diodes can be realized with these highly oriented 2D films. Finally, amplified spontaneous emission with a low threshold 4.16 µJ cm-2 is achieved and distributed feedback lasers are also demonstrated. These results show that it is important to control the morphology of the quasi-2D films to achieve efficient energy transfer, which is a critical requirement for light-emitting devices.

Realization of high-efficiency fluorescent organic light-emitting diodes with low driving voltage.

It is commonly accepted that a full bandgap voltage is required to achieving efficient electroluminescence (EL) in organic light-emitting diodes. In this work, we demonstrated organic molecules with a large singlet-triplet splitting can achieve efficient EL at voltages below the bandgap voltage. The EL originates from delayed fluorescence due to triplet fusion. Finally, in spite of a lower quantum efficiency, a blue fluorescent organic light-emitting diode having a power efficiency higher than some of the best thermally activated delayed fluorescent and phosphorescent blue organic light-emitting diodes is demonstrated. The current findings suggest that leveraging triplet fusion from purely organic molecules in organic light-emitting diode materials offers an alternative route to achieve stable and high efficiency blue organic light-emitting diodes.

Long-Wavelength Lead Sulfide Quantum Dots Sensing up to 2600 nm for Short-Wavelength Infrared Photodetectors.

Lead sulfide nanoparticles (PbS NPs) are used in the short-wavelength infrared photodetectors because of their excellent photosensitivity, band gap tunability, and solution processability. It has been a challenge to synthesize high-quality PbS NPs with an absorption peak beyond 2000 nm. In this work, using PbS seed crystals with an absorption peak at 1960 nm, we report a successful synthesis of very large monodispersed PbS NPs having a diameter up to 16 nm by multiple injections. The resulting NPs have an absorption peak over 2500 nm with a small full width at half-maximum of 24 meV. To demonstrate the applications of such large quantum dots (QDs), broadband heterojunction photodetectors are fabricated with the large PbS QDs of an absorption peak at 2100 nm. The resulting devices have an external quantum efficiency (EQE) of 25% (over 50% internal quantum efficiency) at 2100 nm corresponding to a responsivity of 0.385 A/W and an EQE of ∼60% in the visible range.

Manipulating Refractive Index in Organic Light-Emitting Diodes.

In a conventional organic light-emitting diode (OLED), only a fraction of light can escape to the glass substrate and air. Most radiation is lost to two major channels: waveguide modes and surface plasmon polaritons. It is known that reducing the refractive indices of the constituent layers in an OLED can enhance light extraction. Among all of the layers, the refractive index of the electron transport layer (ETL) has the largest impact on light extraction because it is the layer adjacent to the metallic cathode. Oblique angle deposition (OAD) provides a way to manipulate the refractive index of a thin film by creating an ordered columnar void structure. In this work, using OAD, the refractive index of tris(8-hydroxyquinoline)aluminum (Alq3) can be tuned from 1.75 to 1.45. With this low-index ETL deposited by OAD, the resulting phosphorescent OLED shows nearly 30% increase in light extraction efficiency.