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Transition metal dichalcogenide (TMD) nanosheets exfoliated in the liquid phase are of significant interest owing to their potential for scalable and flexible photoelectronic applications. Although various dispersants such as surfactants, oligomers, and polymers are used to obtain highly exfoliated TMD nanosheets, most of them are electrically insulating and need to be removed; otherwise, the photoelectric properties of the TMD nanosheets degrade. Here, inorganic halide perovskite nanocrystals (NCs) of CsPbX3 (X = Cl, Br, or I) are presented as non-destructive dispersants capable of dispersing TMD nanosheets in the liquid phase and enhancing the photodetection properties of the nanosheets, thus eliminating the need to remove the dispersant. MoSe2 nanosheets dispersed in the liquid phase are adsorbed with CsPbCl3 NCs. The CsPbCl3 nanocrystals on MoSe2 efficiently withdraw electrons from the nanosheets, and suppress the dark current of the MoSe2 nanosheets, leading to flexible near-infrared MoSe2 photodetectors with a high ON/OFF photocurrent ratio and detectivity. Moreover, lanthanide ion-doped CsPbCl3 NCs enhance the ON/OFF current ratio to >106 . Meanwhile, the dispersion stability of the MoSe2 nanosheets exfoliated with the perovskite NCs is sufficiently high.
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Coaxial type piezoelectric energy generator (C-PEG) nanofiber was fabricated by a self-designed continuous electrospinning deposition system. Piezoelectric PVDF-TrFE nanofiber as an electroactive material was electrospun at a discharge voltage of 9-12 kV onto a simultaneously rotating and transverse moving Cu metal wire at an angular velocity of ω g = 60-120 RPM. The piezoelectric coefficient d33 of the PVDF-TrFE nanofiber was approximately -20 pm V-1. The generated output voltage (V G) increased according to the relationship exp(-α P) (α = 0.41- 0.57) as the pressure (P) increased from 30 to 500 kpa. The V G values for ten and twenty pieces of C-PEG were V G = 3.9 V and 9.5 V at P = 100 kpa, respectively, relatively high output voltages compared to previously reported values. The high V G for the C-PEG stems from the fact that it can generate a fairly high V G due to the increased number of voltage collection points compared to a conventional two-dimensional (2-dim) capacitor type of piezoelectric film or fiber device. C-PEG yarn was also fabricated via the dip-coating of a PDMS polymer solution, followed by winding with Ag-coated nylon fiber as an outer electrode. The current and power density of ten pieces of C-PEG yarn were correspondingly 22 nA cm-2 and 8.6 µW cm-3 at V G = 1.97 V, higher than previously reported values of 5.54 and 6 µW cm-3. The C-PEG yarn, which can generate high voltage compared to the conventional film/nanofiber mat type, is expected to be very useful as a wearable energy generator system.
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ZnO nanoparticles (NPs) of 4-5 nm, widely adopted as an electron transport layer (ETL) in quantum dot light emitting diodes (QD-LEDs), were synthesized using the solution-precipitation process. It is notable that synthesized ZnO NPs are highly degenerate intrinsic semiconductors and their donor concentration can be increased up to N D = 6.9 × 1021 cm-3 by annealing at 140 °C in air. An optical bandgap increase of as large as 0.16-0.33 eV by degeneracy is explained well by the Burstein-Moss shift. In order to investigate the influence of intrinsic defects of ZnO NP ETLs on the performance of QD-LED devices without a combined annealing temperature between ZnO NP ETLs and the emissive QD layer, pre-annealed ZnO NPs at 60 °C, 90 °C, 140 °C, and 180 °C were spin-coated on the annealed QD layer without further post-annealing. As the annealing temperature increases from 60 °C to 180 °C, the defect density related to oxygen vacancy (V O) in ZnO NPs is reduced from 34.4% to 17.8%, whereas the defect density of interstitial Zn (Zni) is increased. Increased Zni reduces the width (W) of the depletion region from 0.21 to 0.12 nm and lowers the Schottky barrier (ФB) between ZnO NPs and the Al electrode from 1.19 to 0.98 eV. We reveal for the first time that carrier conduction between ZnO NP ETLs and the Al electrode is largely affected by the concentration of Zni above the conduction band minimum, and effectively described by space charge limited current and trap charge limited current models.
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We have demonstrated a few-layer black phosphorus (BP) phototransistor of stable operation in ambient air environment and at near-infrared light (λ = 1550 nm). The air-stable electronic and optoelectronic properties of the few-layer BP phototransistor have been achieved by a proper Al2O3 passivation. The optical identification method and qualitative and quantitative electrical characterizations of the few-layer BP phototransistor in dark state confirmed that the device performance was robust in ambient air, to further chemical treatments, and storage of more than six months. In addition, the low-frequency noise characterizations had revealed that the noise spectral density related to the sensitivity of phototransistor was reduced. Owing to the suppression of interaction between few-layer BP and adsorbates arising from the Al2O3 passivation, a fast rise time of the few-layer BP phototransistor, less than 100 µs, had been observed, demonstrating the intrinsic photoresponse properties of few-layer BP. The low dark current of â¼4 nA at the operation bias and the reasonable responsivity of â¼6 mA W-1 were obtained under the condition lacking adsorbates interactions. Internally, the dark current and responsivity level was tunable by changing the operation bias. Our results are close to the intrinsic properties of the few-layer BP phototransistor, implying that it can be a building block of functioned few-layer BP photodetectors.
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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 23â¯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.
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Ag nanowire (NW) mesh is used as transparent conducting electrode for high efficient flexible organic solar cells (OSCs). The Ag NW mesh electrode facilitates light scattering and trapping, allowing enhancement of light absorption in the active layer. OSCs incorporating Ag NW mesh electrode exhibit maximum power conversion efficiency (PCE) of 4.47%, 25%, higher than that of OSCs with a conventional ITO electrode (3.63%).
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ZnO, a wide bandgap semiconductor, has attracted much attention due to its multifunctionality, such as transparent conducting oxide, light-emitting diode, photocatalyst, and so on. To improve its performances in the versatile applications, numerous hybrid strategies of ZnO with graphene have been attempted, and various synergistic effects have been achieved in the ZnO-graphene hybrid nanostructures. Here we report extraordinary charge transport behavior in Al-doped ZnO (AZO)-reduced graphene oxide (RGO) nanocomposites. Although the most challenging issue in semiconductor nanocomposites is their low mobilities, the AZO-RGO nanocomposites exhibit single crystal-like Hall mobility despite the large quantity of nanograin boundaries, which hinder the electron transport by the scattering with trapped charges. Because of the significantly weakened grain boundary barrier and the proper band alignment between the AZO and RGO, freely conducting electrons across the nanograin boundaries can be realized in the nanocomposites. This discovery of the structurally nanocrystalline-electrically single crystalline composite demonstrates a new route for enhancing the electrical properties in nanocomposites based on the hybrid strategy.
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Silver (Ag) grid transparent electrode is one of the most promising transparent conducting electrodes (TCEs) to replace conventional indium tin oxide (ITO). We systematically investigate an effect of geometric lattice modifications on optical and electrical properties of Ag grid electrode. The reference Ag grid with 5 µm width and 100 µm pitch (duty of 0.05) prepared by conventional photo-lithography and lift-off processes shows the sheet resistance of 13.27 Ω/sq, transmittance of 81.1%, and resultant figure of merit (FOM) of 129.05. Three different modified Ag grid electrodes with stripe added-mesh (SAM), triangle-added mesh (TAM), and diagonal-added mesh (DAM) are suggested to improve optical and electrical properties. Although all three of SAM, TAM, and DAM Ag grid electrodes exhibit the lower transmittance values of about 72 - 77%, they showed much decreased sheet resistance of 6 - 8 Ω/sq. As a result, all of the lattice-modified Ag grid electrodes display significant improvement of FOM and the highest value of 171.14 is obtained from DAM Ag grid, which is comparable to that of conventional ITO electrode (175.46). Also, the feasibility of DAM Ag gird electrode for use in organic solar cell is confirmed by finite difference time domain (FDTD) simulations. Unlike a conventional ITO electrode, DAM Ag grid electrode can induce light scattering and trapping due to the diffuse transmission that compensates for the loss in optical transparency, resulting in comparable light absorption in the photo active layer of poly(3-hexylthiophene) (P3HT): [6,6]-phenyl-C61-butyric acid methyl ester (PC60BM). P3HT:PC60BM based OSCs with the DAM Ag grid electrode were fabricated, which also showed the potential for ITO-free transparent electrode.
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A facile thin film encapsulation (TFE) method having a triple-layered structure of a-SiN x :H/SiO x N y /hybrid SiO x (ASH) on QD-LEDs was performed utilizing both reproducible plasma-enhanced chemical vapor deposition (PECVD) and simple dip-coating processes without adopting atomic layer deposition (ALD). The ASH films fabricated on a polyethylene terephthalate (PET) substrate show a high average transmittance of 88.80% in the spectral range of 400-700 nm and a water vapor transmission rate (WVTR) value of 7.3 × 10-4 g per m2 per day. The measured time to reach 50% of the initial luminance (T50) at initial luminance values of 500, 1000, and 2000 cd m-2 was 711.6, 287.7, and 78.6 h, respectively, and the extrapolated T50 at 100 cd m-2 is estimated to be approximately 9804 h, which is comparable to that of the 12 112 h for glass lid-encapsulated QD-LEDs. This result demonstrates that TFE with the ASH films has the potential to overcome the conventional drawbacks of glass lid encapsulation.
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The widely used ZnO quantum dots (QDs) as an electron transport layer (ETL) in quantum dot light-emitting diodes (QLEDs) have one drawback. That the balancing of electrons and holes has not been effectively exploited due to the low hole blocking potential difference between the valence band (VB) (6.38 eV) of ZnO ETL and (6.3 eV) of CdSe/ZnS QDs. In this study, ZnO QDs chemically reacted with capping ligands of oleic acid (OA) to decrease the work function of 3.15 eV for ZnO QDs to 2.72~3.08 eV for the ZnO-OA QDs due to the charge transfer from ZnO to OA ligands and improve the efficiency for hole blocking as the VB was increased up to 7.22~7.23 eV. Compared to the QLEDs with a single ZnO QDs ETL, the ZnO-OA/ZnO QDs double ETLs optimize the energy level alignment between ZnO QDs and CdSe/ZnS QDs but also make the surface roughness of ZnO QDs smoother. The optimized glass/ITO/PEDOT:PSS/PVK//CdSe/ZnS//ZnO-OA/ZnO/Ag QLEDs enhances the maximum luminance by 5~9% and current efficiency by 16~35% over the QLEDs with a single ZnO QDs ETL, which can be explained in terms of trap-charge limited current (TCLC) and the Fowler-Nordheim (F-N) tunneling conduction mechanism.
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We present data, which were obtained before bending and after bending, for the electrical bistabilities, memory stabilities, and memory mechanisms of three-layer structured flexible bistable organic memory (BOM) devices, which were fabricated utilizing the ultrathin graphite sheets (UGS) sandwiched between insulating poly(methylmethacrylate) (PMMA) polymer layers. The UGS were formed by transferring UGS (about 30 layers) and using a simple spin-coating technique. Transmission electron microscopy (TEM) measurements were performed to investigate the microstructural properties of the PMMA/UGS/PMMA films. Current-voltage (I-V) measurements were carried out to investigate the electrical properties of the BOM devices containing the UGS embedded in the PMMA polymer. Current-time (I-t) and current-cycle measurements under flat and bent conditions were performed to investigate the memory stabilities of the BOM devices. The memory characteristics of the BOM maintained similar device efficiencies after bending and were stable during repeated bendings of the BOM devices. The mechanisms for these characteristics of the fabricated BOM are described on the basis of the I-V results.
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The electrical properties of flexible nonvolatile organic bistable devices (OBDs) fabricated with graphene sandwiched between two insulating poly(methyl methacrylate) (PMMA) polymer layers were investigated. Current-voltage (I-V) measurements on the Al/PMMA/graphene/PMMA/indium-tin-oxide/poly(ethylene terephthalate) devices at 300 K showed a current bistability due to the existence of the graphene, indicative of charge storage in the graphene. The maximum ON/OFF ratio of the current bistability for the fabricated OBDs was as large as 1 x 10(7), and the endurance number of ON/OFF switchings was 1.5 x 10(5) cycles, and an ON/OFF ratio of 4.4 x 10(6) was maintained for retention times larger than 1 x 10(5) s. No interference effect was observed for the scaled-down OBDs containing a graphene layer. The memory characteristics of the OBDs maintained similar device efficiencies after bending and were stable during repetitive bendings of the OBDs. The mechanisms for these characteristics of the fabricated OBDs are described on the basis of the I-V results.
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Halide vacancy defect is one of the major origins of non-radiative recombination in the lead halide perovskite light emitting devices (LEDs). Hence the defect passivation is highly demanded for the high-performance perovskite LEDs. Here, we demonstrated that FA doping led to the enrichment of Br in Cs1-xFAxPbBr3 QDs. Due to the defect passivation by the enriched Br, the trap density in Cs1-xFAxPbBr3 significantly decreased after FA doping, and which improved the optical properties of Cs1-xFAxPbBr3 QDs and their QD-LEDs. PLQY of Cs1-xFAxPbBr3 QDs increased from 76.8% (x = 0) to 85.1% (x = 0.04), and Lmax and CEmax of Cs1-xFAxPbBr3 QD-LEDs were improved from Lmax = 2880 cd m-2 and CEmax = 1.98 cd A-1 (x = 0) to Lmax = 5200 cd m-2 and CEmax = 3.87 cd A-1 (x = 0.04). Cs1-xFAxPbBr3 QD-LED device structure was optimized by using PVK as a HTL and ZnO modified with b-PEI as an ETL. The energy band diagram of Cs1-xFAxPbBr3 QD-LEDs deduced by UPS analyses.
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Zn-doped SnOx/Ag/Zn-doped SnOx(ZTO/Ag/ZTO) multilayer thin films fabricated on a polyethylene terephthalate (PET) substrate using an optimized N2-to-(Ar + O2) gas ratio are used for transparent thin-film heaters with high performance and chemical stability. The ZTO/Ag/ZTO-based multilayer thin film exhibits enhanced durability at high temperatures and humid environments by incorporating nitrogen. The bending test results-there was no significant change in the sheet resistance even after 10,000 bending cycles-highlight the mechanical flexibility of the ZTO/Ag/ZTO multilayer thin film. The ZTO/Ag/ZTO-based thin-film heater on PET, fabricated under optimized deposition gas conditions, exhibits a fast thermal response time of 30 s and a low driving voltage of 6 V to attain 100 °C. It also exhibits uniform heat distribution at saturated temperature and chemical stability after 100 heating-cooling cycles. Hence, the proposed ZTO/Ag/ZTO-based thin-film heater is applicable for use in front and rear window automobile and building applications.
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Owing to the growth of demand for highly integrated electronic devices, high heat dissipation of thermal management materials is essential. Epoxy composites have been prepared with vertically aligned (VA) three-dimensional (3D)-structured SiC sheet scaffolds. The required VA-SiC sheet scaffolds were prepared by a novel approach starting with a graphene oxide (GO) scaffold. The VA-GO scaffolds were reduced to VA-graphene scaffolds in an argon environment, and the latter were subsequently transformed into VA-SiC sheet scaffolds by a template-assisted chemical vapor deposition method. Epoxy resin was filled in the empty spaces of the 3D scaffold of SiC sheets to prepare the composite mass. The material so prepared shows anisotropic thermal property with ultrahigh through-plane conductivity of 14.32 W·m-1·K-1 at a SiC sheet content of 3.71 vol %. A thermal percolation is observed at 1.78 vol % SiC filler. The SiC sheet scaffold of covalently interconnected SiC nanoparticles plays a vital role in the formation of the thermal conductive network to significantly enhance the thermal conductivity of epoxy composites. The application of the VA-SiC/epoxy composite as an efficient thermal dissipating material has also been presented. The VA-SiC/epoxy composites have a strong potential for preparing heat-dissipating components in integrated microelectronics.
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All-solid-state thin-film batteries have been actively investigated as a power source for various microdevices. However, insufficient research has been conducted on thin-film encapsulation, which is an essential element of these batteries as solid electrolytes and Li anodes are vulnerable to moisture in the atmosphere. In this study, a hybrid thin-film encapsulation structure of hybrid SiOy/SiNxOy/a-SiNx:H/Parylene is suggested and investigated. The water-vapor transmission rate of hybrid thin-film encapsulation is estimated to be 4.9 × 10-3 g m-2·day-1, a value that is applicable to batteries as well as flexible solar cells, thin-film transistor liquid-crystal display, and E-papers. As a result of hybrid thin-film encapsulation, it is confirmed that the all-solid-state thin-film batteries are stable even after 100 charge/discharge cycles in the air atmosphere for 30 days and present a Coulombic efficiency of 99.8% even after 100 cycles in the air atmosphere. These results demonstrate that the thin-film encapsulation structure of hybrid SiOy/SiNxOy/a-SiNx:H/Parylene can be employed in thin-film batteries while retaining long-term stability.
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Organic electronic devices such as organic light-emitting diodes (OLEDs), quantum dot LEDs, and organic photovoltaics are promising technologies for future electronics. However, achieving long-term stability of organic-based optoelectronic devices has been regarded as a crucial problem to be solved. In this work, a simple and reproducible fabrication method for ultralow water permeation barrier films having a triple-layered (triad) hydrogenated silicon nitride (a-SiNx:H)/nanosilicon oxynitride (n-SiOxNy)/hybrid silicon oxide (h-SiOx) multistructure is presented. Two triad (a-SiNx:H/n-SiOxNy/h-SiOx)n=2 multistructure barrier films are deposited on both sides of a poly(ethylene terephthalate) substrate using a combination of low-pressure plasma-enhanced chemical vapor deposition and dip coating. The deposited films show a high average transmittance (400-700 nm) of 84% and an ultralow water vapor transmission rate of 2 × 10-6 g/m2/day. In the electroluminescence characteristics of OLEDs encapsulated with two triad barrier films, the operational lifetime (T50) of OLEDs is 1584 h, which is almost similar to that (1416 h) of OLEDs encapsulated with a glass lid.
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In modern society, advanced technology has facilitated the emergence of multifunctional appliances, particularly, portable electronic devices, which have been growing rapidly. Therefore, flexible thermally conductive materials with the combination of properties like outstanding thermal conductivity, excellent electrical insulation, mechanical flexibility, and strong flame retardancy, which could be used to efficiently dissipate heat generated from electronic components, are the demand of the day. In this study, graphite fluoride, a derivative of graphene, was exfoliated into graphene fluoride sheets (GFS) via the ball-milling process. Then, a suspension of graphene oxide (GO) and GFSs was vacuum-filtrated to obtain a mixed mass, and subsequently, the mixed mass was subjected to reduction under the action hydrogen iodide at low temperature to transform the GO to reduced graphene oxide (rGO). Finally, a highly flexible and thermally conductive 30-µm thick GFS@rGO hybrid film was prepared, which showed an exceptional in-plane thermal conductivity (212 W·m-1·K-1) and an excellent electrical insulating property (a volume resistivity of 1.1 × 1011 Ω·cm). The extraordinary in-plane thermal conductivity of the GFS@rGO hybrid films was attributed to the high intrinsic thermal conductivity of the filler components and the highly ordered filler alignment. Additionally, the GFS@rGO films showed a tolerance to bending cycles and high-temperature flame. The tensile strength and Young's modulus of the GFS@rGO films increased with increasing the rGO content and reached a tensile strength of 69.3 MPa and a Young's modulus of 10.2 GPa at 20 wt % rGO. An experiment of exposing the films to high-temperature flame demonstrated that the GFS@rGO films could efficiently prevent fire spreading. The microcombustion calorimetry results indicated that the GFS@rGO had significantly lower heat release rate (HRR) compared to the GO film. The peak HRR of GFS@rGO10 was only 21 W·g-1 at 323 °C, while that of GO was 198 W·g-1 at 159 °C.
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Despite the great interest in inorganic halide perovskites (IHPs) for a variety of photoelectronic applications, environmentally robust nanopatterns of IHPs have hardly been developed mainly owing to the uncontrollable rapid crystallization or temperature and humidity sensitive polymorphs. Herein, we present a facile route for fabricating environment- and phase-stable IHP nanopatterns over large areas. Our method is based on nanoimprinting of a soft and moldable IHP adduct. A small amount of poly(ethylene oxide) was added to an IHP precursor solution to fabricate a spin-coated film that is soft and moldable in an amorphous adduct state. Subsequently, a topographically prepatterned elastomeric mold was used to nanoimprint the film to develop well-defined IHP nanopatterns of CsPbBr3 and CsPbI3 of 200 nm in width over a large area. To ensure environment- and phase-stable black CsPbI3 nanopatterns, a polymer backfilling process was employed on a nanopatterned CsPbI3. The CsPbI3 nanopatterns were overcoated with a thin poly(vinylidene fluoride-co-trifluoroethylene) (PVDF-TrFE) film, followed by thermal melting of PVDF-TrFE, which formed the air-exposed CsPbI3 nanopatterns laterally confined with PVDF-TrFE. Our polymer backfilled CsPbI3 nanopatterns exhibited excellent environmental stability over one year at ambient conditions and for 10 h at 85 °C, allowing the development of arrays of two-terminal, parallel-type photodetectors with nanopatterned photoactive CsPbI3 channels. Our polymer-assisted nanoimprinting offers a fast, low-pressure/temperature patterning method for high-quality nanopatterns on various substrates over a large area, overcoming conventional costly time-consuming lithographic techniques.
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A hybrid polymer-nanocrystal (NC) light-emitting diode (LED) device with a single active layer structure is simply fabricated by a spin coating. From a high-resolution transmission electron microscopy (HRTEM) study, each PVK polymer particle is observed to be capped with TPBi molecules and CdSe/ZnS NCs are mainly distributed along the circumference of PVK and TPBi surfaces, resulting in a core-shell polymer-NC hybrid of [CdSe/ZnS]/TPBi/[CdSe/ZnS]/PVK. An Al/[CdSe/ZnS]/TPBi/[CdSe/ZnS]/PVK/indium-tin oxide(ITO)/glass LED shows electroluminescence (EL) centered at around 585 nm at the forward bias of +10 V, which clearly reveals that CdSe/ZnS NCs existing at the interface between PVK and TPBi act as recombination centers for excitons. In particular, EL can be observed at both forward bias and reverse bias, and this means that this device with an isotropic distribution of NCs has an inversion symmetry.