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1.
Adv Mater ; 35(9): e2207617, 2023 Mar.
Article in English | MEDLINE | ID: mdl-36353914

ABSTRACT

Mixed-cation hybrid perovskite nanocrystal (HPNC) with high crystallinity, color purity, and tunable optical bandgap offers a practical pathway toward next-generation displays. Herein, a two-step modified hot-injection combined with cation compositional engineering and surface treatment to synthesize high-purity cesium/formamidinium lead bromide HPNCs(Cs1-x FAx PbBr3 ) is presented. The optimized Cs0.5 FA0.5 PbBr3 light-emitting devices (LEDs) exhibit uniform luminescence of 3500 cd m-2 and a prominent current efficiency of 21.5 cd A-1 . As a proof of concept, a self-healing polymer (SHP) integrated with white LED backlight and laser prototypes exhibited 4 h autonomous self-healing through the synergistic effect of weak reversible imine bonds and stronger H-bonds. First, the SHP-HPNCs-initial and SHP-HPNCs-cut possess high long-term stability and dramatically suppressed lead leakage as low as 0.6 ppm along with a low leakage rate of 1.11 × 10-5 cm2 and 3.36 × 10-5 cm2 even over 6 months in water. Second, the Cs0.5 FA0.5 PbBr3 HPNCs and SHP-induced shattered-repaired perovskite glass substrate show the lowest lasing threshold values of 1.24 and 8.58 µJ cm-2 , respectively. This work provides an integrative and in-depth approach to exploiting SHP with intrinsic and entropic self-healing capabilities combined with HPNCs to develop robust and reliable soft-electronic backlight and laser applications.

2.
J Am Chem Soc ; 144(46): 21146-21156, 2022 11 23.
Article in English | MEDLINE | ID: mdl-36346318

ABSTRACT

As a crystal approaches a few nanometers in size, atoms become nonequivalent, bonds vibrate, and quantum effects emerge. To study quantum dots (QDs) with structural control common in molecular science, we need atomic precision synthesis and analysis. We describe here the synthesis of lead bromide perovskite magic-sized nanoclusters via self-organization of a lead malate chelate complex and PbBr3- under ambient conditions. Millisecond and angstrom resolution electron microscopic analysis revealed the structure and the dynamic behavior of individual QDs─structurally uniform cubes made of 64 lead atoms, where eight malate molecules are located on the eight corners of the cubes, and oleylammonium cations lipophilize and stabilize the edges and faces. Lacking translational symmetry, the cube is to be viewed as a molecule rather than a nanocrystal. The QD exhibits quantitative photoluminescence and stable electroluminescence at ≈460 nm with a narrow half-maximum linewidth below 15 nm, reflecting minimum structural defects. This controlled synthesis and precise analysis demonstrate the potential of cinematic chemistry for the characterization of nanomaterials beyond the conventional limit.


Subject(s)
Nanoparticles , Nanostructures , Quantum Dots , Quantum Dots/chemistry , Malates
3.
ACS Appl Mater Interfaces ; 14(15): 17691-17697, 2022 Apr 20.
Article in English | MEDLINE | ID: mdl-35411769

ABSTRACT

Perovskite quantum dots (PQDs) are applicable in light-emitting diodes (LEDs) owing to their color tunability, high color purity, and excellent photoluminescence quantum yield (PLQY) in the solution state. However, a PQD film obtained through nonradiative recombination by concentration quenching and the formation of surface defects exhibited a low PLQY. In this study, we focused on the energy transfer between PQDs with different energy gaps (Eg) to reduce nonradiative recombination in the film state and consequently achieve high device performance. We prepared size-controlled PQDs measuring 10.7 nm (large-size QD; LQD) and 7.9 nm (small-size QD; SQD) with different Eg values and observed a spectral overlap between SQD emission and LQD absorption. To investigate the Förster resonance energy transfer (FRET) from SQDs to LQDs, we prepared SQD-LQD mixed QDs (MQDs). The MQD film enhanced LQD emission and exhibited a higher PLQY (52%) with a longer PL decay time (7.4 ns) than those exhibited by the neat LQD film (38% and 6.2 ns). This energy transfer was determined to be FRET by photoluminescence excitation and PL decay times. Moreover, the external quantum efficiency of an MQD-based LED increased to 15%, indicating that the FRET process can enhance the PLQY of the film and LED efficiency.

4.
Sci Rep ; 12(1): 4620, 2022 Mar 17.
Article in English | MEDLINE | ID: mdl-35301429

ABSTRACT

The emergence of green materials has attracted considerable attention in the field of optoelectronics. Copper-based lead-free metal halide (with a near-unity quantum yield) obtained from Cs3Cu2I5 nanocrystals (NCs) can exhibit blue emission with a wavelength of 440 nm and provide outstanding stability for various applications. However, in practical applications, colloidal dispersion purity and film quality are inadequate toward a high-performance device. In this study, antisolvent-free gel permeation chromatography is used to purify Cs3Cu2I5 NCs. The purified Cs3Cu2I5 NCs exhibit a high photoluminescent quantum yield and provide a highly oriented single-crystal film. Density functional theory calculation results indicate that the iodide-rich surface in the NCs makes them highly stable. In addition, it has been demonstrated for the first time that the mixture of polymethyl methacrylate (PMMA) and Cs3Cu2I5 NCs has waterproofing capabilities. The composite film consisting of Cs3Cu2I5 NCs and PMMA can survive in water for several days. This result opens up more possibilities for the application of these green material.

5.
Article in English | MEDLINE | ID: mdl-35076204

ABSTRACT

Metal halide perovskites attract significant attention because of their excellent optoelectronic and semiconducting properties. However, there are environmental concerns related to the toxicity of the lead metal that is mainly used in these perovskites. PEA2SnI4 perovskite is a potential candidate for lead-free perovskites because of its pure red emission. Although, undesired Sn4+ oxidation results in the deterioration of PEA2SnI4 perovskite. We demonstrate the two-step crystallization of PEA2SnI4 through the (i) reprecipitation and (ii) recrystallization processes. A film prepared using this method exhibits narrowed emission, with a full width at half-maximum from 30.0 to 26.1 nm, because of its homogeneous emission. Moreover, the Sn4+ content of two-step-crystallized PEA2SnI4 films is five times lower than that of a control film. Diffusion-ordered spectroscopy analysis indicates that the two-step precursor exhibits a smaller hydrodynamic radius crystal seed, which enhances crystallization during spin coating. The resulting two-step crystallized PEA2SnI4-based light-emitting diode (LED) exhibits a maximum external quantum efficiency (EQE) of 0.4% with an average of 0.2%, which is two times greater than that of the control device. This two-step approach may be generalized to synthesize other lead-free materials.

6.
Cerebrovasc Dis Extra ; 11(2): 61-68, 2021.
Article in English | MEDLINE | ID: mdl-34034253

ABSTRACT

INTRODUCTION: During exposure of the carotid arteries, embolism from the surgical site is recognized as a primary cause of neurological deficits or new cerebral ischemic lesions following carotid endarterectomy (CEA), and associations have been reported between histological neovascularization in the carotid plaque and both plaque vulnerability and the development of artery-to-artery embolism. Superb microvascular imaging (SMI) enables accurate visualization of neovessels in the carotid plaque without the use of intravenous contrast. This study aimed to determine whether preoperative SMI ultrasound for cervical carotid artery stenosis predicts the development of microembolic signals (MES) on transcranial Doppler (TCD) during exposure of the carotid arteries in CEA. METHODS: Preoperative cervical carotid artery SMI ultrasound followed by CEA under TCD monitoring of MES in the ipsilateral middle cerebral artery was conducted in 70 patients previously diagnosed with internal carotid artery stenosis (defined as ≥70%). First, observers visually identified intraplaque microvascular flow (IMVF) signals as moving enhancements located near the surface of the carotid plaque within the plaque on SMI ultrasonograms. Next, regions of interest (ROI) were manually placed at the identified IMVF signals (or at arbitrary places within the plaque when no IMVF signals were identified within the carotid plaque) and the carotid lumen, and time-intensity curves of the IMVF signal and lumen ROI were generated. Ten heartbeat cycles of both time-intensity curves were segmented into each heartbeat cycle based on gated electrocardiogram findings and averaged with respect to the IMVF signal and lumen ROI. The difference between the maximum and minimum intensities (ID) was calculated based on the averaged IMVF signal (IDIMVF) and lumen (IDl) curves. Finally, the ratio of IDIMVF to IDl was calculated. RESULTS: MES during exposure of the carotid arteries were detected in 17 patients (24%). The incidence of identification of IMVF signals was significantly greater in patients with MES (94%) than in those without (57%; p = 0.0067). The IDIMVF/IDl ratio was significantly greater in patients with MES (0.108 ± 0.120) than in those without (0.017 ± 0.042; p < 0.0001). The specificity and positive predictive value for the IDIMVF/IDl ratio for prediction of the development of MES were significantly higher than those for the identification of IMVF signals. Logistic regression analysis revealed that only the IDIMVF/IDl ratio was significantly associated with the development of MES (95% CI 101.1-3,628.9; p = 0.0048). CONCLUSION: Preoperative cervical carotid artery SMI ultrasound predicts the development of MES on TCD during exposure of the carotid arteries in CEA.


Subject(s)
Carotid Stenosis/surgery , Endarterectomy, Carotid , Intracranial Embolism/diagnostic imaging , Microvessels/diagnostic imaging , Middle Cerebral Artery/diagnostic imaging , Ultrasonography, Doppler, Transcranial , Ultrasonography , Aged , Aged, 80 and over , Carotid Stenosis/complications , Carotid Stenosis/diagnostic imaging , Endarterectomy, Carotid/adverse effects , Female , Humans , Image Interpretation, Computer-Assisted , Intracranial Embolism/etiology , Male , Middle Aged , Predictive Value of Tests , Preoperative Care , Risk Assessment , Risk Factors , Treatment Outcome
7.
ACS Appl Mater Interfaces ; 12(48): 53891-53898, 2020 Dec 02.
Article in English | MEDLINE | ID: mdl-33210903

ABSTRACT

Metal halides doping of perovskite nanocrystals (NCs) has been shown to precisely control nonradiative pathways and to improve photoluminescence quantum yield (PLQY). Here, we report a trivalent lanthanide halide neodymium (III) chloride (NdCl3)-doped perovskite NCs prepared with a post-synthetic room temperature treatment for efficient blue light-emitting devices (LEDs). The Nd 3d and Cl 2p core peaks were observed in the NdCl3-doped NCs, which allowed for simultaneous doping of Nd3+ and Cl- into the pristine CsPbBr3 NCs. The NdCl3-doped NCs exhibited blue emission at a peak wavelength of 478 nm with a high PLQY of 97% in solution. We found that the Nd3+ cation incorporated into the NCs more effectively suppressed nonradiative recombination compared with common halide anion exchange from temperature dependence of optical properties. Blue LEDs based on NdCl3-doped NCs had an external quantum efficiency of 2.7%, which represents a considerable performance improvement compared with LEDs based on organic chloride salt-doped NCs.

8.
ACS Appl Mater Interfaces ; 12(40): 45574-45581, 2020 Oct 07.
Article in English | MEDLINE | ID: mdl-32914951

ABSTRACT

The surface modification of metal halide perovskite nanocrystals (NCs) significantly impacts their optical properties and colloidal stability. This subsequently affects the performance of light-emitting devices (LEDs). Therefore, numerous surface passivation techniques like ligand exchange and metal halide doping have been explored to passivate the surface defects of perovskite NCs and obtain highly efficient LEDs. In this study, we demonstrated the postsynthetic metal halide doping treatment using lead(II) bromide (PbBr2) to passivate the surface defects of the CsPbBr3 NCs at a moderate reaction temperature of 80 °C. The alkyl quaternary ammonium salt, didodecyldimethylammonium bromide (DC12AB), enabled the complete dissolution of PbBr2 in a nonpolar solvent, toluene. Because of surface crystal growth, the particle sizes of the PbBr2-doped CsPbBr3 NCs were higher than those of the as-synthesized CsPbBr3 NCs. The photoluminescence quantum yield of the CsPbBr3 NCs drastically increased from 26.8 to 83.9% after the PbBr2 doping treatment. Moreover, the PbBr2-doped CsPbBr3 NCs possessed long-term colloidal stability of more than 2 months that indicates the strong bonding between the NCs and ligands. We observed that the alkyl chain length of the quaternary alkyl ammonium salts affected the luminance and device stability during operations. In this study, a promising strategy was devised to achieve highly luminescent perovskite NCs with excellent colloidal stability that can enhance the performance of LEDs.

9.
ACS Appl Mater Interfaces ; 11(28): 25351-25357, 2019 Jul 17.
Article in English | MEDLINE | ID: mdl-31259510

ABSTRACT

For efficient electron injection, a method to control the work functions (WFs) of ZnO electrodes in organic light-emitting devices (OLEDs) is reported in this study. First, ZnO was modified by doping of tetraalkylammonium salts (TRAX) into polyethylenimine ethoxylated (PEIE) for the WF control. Tetrabutylammonium salts (TBAX), where X = chloride, bromide, iodide, acetate, thiocyanate, and tetrafluoroborate anions, were doped into PEIE. A WF of nondoped PEIE-modified ZnO was 3.65 eV, whereas TBAX-doped PEIE-modified ZnO exhibited WFs ranging from 3.52 to 3.00 eV depending on the anion. TBAX salts exhibited different electron-donating capabilities depending on the anion, and the doping of TBAX with a large electron-donating capability exhibited a large WF reduction effect. In addition, tetraethyl- and tetrahexylammonium chlorides were doped into PEIE. PEIE doped with TRACl containing long alkyl chains exhibited a large WF reduction effect due to its low electron-accepting capabilities. In addition, the WF reduction mechanism was considered by the depth direction analysis of the PEIE:TBAX films. Finally, the ZnO/PEIE:TRAX bilayers were applied as electron injection layers in poly[2-methoxy-5-(2-ethylhexyloxy)-1,4-phenylenevinylene] emissive-layer-based OLEDs with an inverted structure. The ZnO/PEIE:TBAX devices with low WFs exhibited low driving voltages.

10.
Adv Mater ; 31(18): e1808300, 2019 May.
Article in English | MEDLINE | ID: mdl-30848005

ABSTRACT

Use of the intrinsic optoelectronic functions of organic semiconductor films has not yet reached its full potential, mainly because of the primitive methodology used to control the molecular aggregation state in amorphous films during vapor deposition. Here, a universal molecular engineering methodology is presented to control molecular orientation; this methodology strategically uses noncovalent, intermolecular weak hydrogen bonds in a series of oligopyridine derivatives. A key is to use two bipyridin-3-ylphenyl moieties, which form self-complementary intermolecular weak hydrogen bonds, and which do not induce unfavorable crystallization. Another key is to incorporate a planar anisotropic molecular shape by reducing the steric hindrance of the core structure for inducing π-π interactions. These synergetic effects enhance horizontal orientation in amorphous organic semiconductor films and significantly increasing electron mobility. Through this evaluation process, an oligopyridine derivative is selected as an electron-transporter, and successfully develops highly efficient and stable deep-red organic light-emitting devices as a proof-of-concept.

11.
Neurol Res ; 41(5): 480-487, 2019 May.
Article in English | MEDLINE | ID: mdl-30774013

ABSTRACT

OBJECTIVE: Adult patients with ischemic moyamoya disease (MMD) who receive treatment with antiplatelet drugs reportedly show improvements in neuropsychological test scores after around 2 years. The purpose of the present study subanalyzing the same patient cohort used in a previous study was to determine which antiplatelet drug, clopidogrel or cilostazol, results in better improvement of cognitive function among non-surgical adult patients showing ischemic MMD without severe hemodynamic compromise. METHODS: Sixty-six patients without cerebral misery perfusion on 15O gas positron emission tomography were treated with pharmacotherapy alone. Patients ≥50 years old and <50 years old initially received clopidogrel and cilostazol, respectively. Any patient suffering side effects of the antiplatelet drug switched to the other antiplatelet drug. Neuropsychological tests were performed at study entry and at the end of the 2-year follow-up, and differences in each neuropsychological test score between the two time points (second test score - first test score) were calculated and defined as Δ scores. RESULTS: Among the five neuropsychological tests, Δ scores for two tests were significantly greater in patients treated with cilostazol (n = 36) than in those treated with clopidogrel (n = 30), and Δ scores of the remaining three tests did not differ between patient groups. Based on Δ scores, 15 patients (23%) were defined as showing interval cognitive improvement. On multivariate analysis, cilostazol administration (95% confidence interval, 1.19-193.98; P = 0.0361) represented an independent predictor of interval cognitive improvement. CONCLUSIONS: Cilostazol may improve cognition better than clopidogrel in non-surgical adult patients with ischemic MMD.


Subject(s)
Cilostazol/pharmacology , Clopidogrel/pharmacology , Cognition/drug effects , Moyamoya Disease/drug therapy , Moyamoya Disease/psychology , Nootropic Agents/therapeutic use , Adult , Female , Follow-Up Studies , Humans , Male , Middle Aged , Prospective Studies , Treatment Outcome
12.
J Stroke Cerebrovasc Dis ; 27(11): 3373-3379, 2018 Nov.
Article in English | MEDLINE | ID: mdl-30174225

ABSTRACT

BACKGROUND AND PURPOSE: Adult patients with symptomatically ischemic moyamoya disease (MMD) initially undergo medical treatment alone including antiplatelet drugs when symptomatic cerebral hemispheres do not exhibit hemodynamic compromise. The purpose of the present study subanalyzing the same patient cohort used in a previous study was to determine which antiplatelet drug, clopidogrel or cilostazol, provides better improvement of cerebral perfusion in such patients. METHODS: All patients without cerebral misery perfusion on 15O gas positron emission tomography (PET) did not undergo revascularization surgery and were treated with medication alone, including antiplatelet therapy. Patients ≥50years and <50years initially received clopidogrel and cilostazol, respectively. When a patient suffered side effects of an antiplatelet drug, they were switched to the other antiplatelet drug. Cerebral blood flow (CBF) in the symptomatic hemisphere was measured at inclusion and at 2years after inclusion using 15O gas PET. RESULTS: Of 68 patients, 31 and 38 were treated with clopidogrel and cilostazol, respectively, for 2years after inclusion. For patients treated with clopidogrel, CBF did not differ between first and second PET. For patients treated with cilostazol, CBF was significantly greater in the second PET than in the first PET. On multivariate analysis, cilostazol administration was an independent predictor of CBF improvement in the symptomatic hemisphere (95% confidence interval, 1.34-139.20; P =.0271). CONCLUSIONS: Cilostazol improves cerebral perfusion better than clopidogrel in adult patients with symptomatically ischemic MMD not accompanied by misery perfusion.


Subject(s)
Brain Ischemia/drug therapy , Cerebrovascular Circulation/drug effects , Moyamoya Disease/drug therapy , Platelet Aggregation Inhibitors/therapeutic use , Tetrazoles/therapeutic use , Ticlopidine/analogs & derivatives , Adult , Blood Flow Velocity , Brain Ischemia/diagnostic imaging , Brain Ischemia/physiopathology , Cilostazol , Clopidogrel , Drug Substitution , Female , Humans , Male , Middle Aged , Moyamoya Disease/diagnostic imaging , Moyamoya Disease/physiopathology , Multivariate Analysis , Oxygen Radioisotopes/administration & dosage , Perfusion Imaging/methods , Platelet Aggregation Inhibitors/adverse effects , Positron-Emission Tomography , Prospective Studies , Radiopharmaceuticals/administration & dosage , Tetrazoles/adverse effects , Ticlopidine/adverse effects , Ticlopidine/therapeutic use , Time Factors , Treatment Outcome
13.
Sci Rep ; 8(1): 11472, 2018 Jul 31.
Article in English | MEDLINE | ID: mdl-30065248

ABSTRACT

The rapid development of organic optoelectronic devices such as organic photovoltaics (OPVs) and organic light-emitting devices (OLEDs) is largely attributable to their advantageous properties of their large area, ultrathin thickness, flexiblility, transparency, and solution processability. Herein, we fabricate and characterize a dual mode OPV-OLED device with three-terminal structure comprising a polymer-based bulk-heterojunction inverted OPV unit and a top-emission white phosphorescent OLED unit back-to-back connected via intermediate metal alloy electrode. Sputter-deposited indium tin oxide was used as a transparent cathode of the inverted OPV unit, whereas Ag-doped Al served as a common OPV/OLED anode, allowing the decoupling of electricity generation and light mission functions. Notably, the doping of Al by Ag facilitated the reduction of surface roughness, allowing the above electrode to be used as a common anode and dramatically reducing the leakage current. Finally, the top-emission OLED unit featured an ultrathin layer of Ag-doped Mg as a semitransparent cathode. Thus, successful integration of the OPV-OLED elements results in the decoupling of electricity generation and light emission functionalities, achieving a power conversion efficiency of 3.4% and an external quantum efficiency of 9.9%.

14.
Ann Nucl Med ; 32(9): 611-619, 2018 Nov.
Article in English | MEDLINE | ID: mdl-30030783

ABSTRACT

OBJECTIVE: The purpose of the present study was to determine how accurately relative cerebral blood flow (RCBF) and relative cerebrovascular reactivity (RCVR) to acetazolamide assessed using brain perfusion single-photon emission computed tomography (SPECT) detected misery perfusion identified on positron emission tomography (PET) in adult patients with ischemic moyamoya disease (MMD). METHODS: Oxygen extraction fraction (OEF), RCBF, and RCVR were assessed using 15O gas PET and N-isopropyl-p-[123I]-iodoamphetamine SPECT without and with acetazolamide challenge, respectively, in 45 patients. Regions of interest (ROIs) were automatically placed in the five middle cerebral artery (MCA) territories in the symptomatic cerebral hemisphere and in the ipsilateral cerebellar hemisphere using a three-dimensional stereotaxic ROI template. For RCBF and RCVR to acetazolamide, the ratio of the MCA ROI to cerebellar ROI was calculated. Of the five MCA ROIs in the symptomatic cerebral hemisphere in each patient, the ROI with the highest and lowest OEF value (two ROIs per patient) was selected for analyses. RESULTS: A significant square or linear correlation was observed between the OEF and RCBF (correlation coefficient, 0.780) or RCVR (correlation coefficient, - 0.345), respectively. The area under the receiver operating characteristic curve for detecting misery perfusion (OEF > 51.3%) was significantly greater for the RCBF than for the RCVR (difference between areas, 0.221; p < 0.0001). Sensitivity, specificity, and positive- and negative-predictive values for the RCBF for detecting misery perfusion were 100, 91, 67, and 100%, respectively. The specificity and positive-predictive value did not differ between the combination of the RCBF and RCVR and the CBF ratio alone. CONCLUSIONS: RCBF assessed using brain perfusion SPECT detects misery perfusion with high sensitivity, a high negative-predictive value, and a low positive-predictive value in adult patients with ischemic MMD. The accuracy of RCVR to acetazolamide assessed using brain perfusion SPECT is lower than that of RCBF.


Subject(s)
Brain Ischemia/complications , Brain/blood supply , Brain/diagnostic imaging , Moyamoya Disease/diagnostic imaging , Moyamoya Disease/physiopathology , Perfusion Imaging , Tomography, Emission-Computed, Single-Photon , Adult , Female , Humans , Male , Middle Aged , Moyamoya Disease/complications , Sensitivity and Specificity
15.
ACS Appl Mater Interfaces ; 10(33): 27885-27893, 2018 Aug 22.
Article in English | MEDLINE | ID: mdl-30047719

ABSTRACT

We report in this article the application of calcium niobate (CNO) perovskite nanosheets for electron injection layers (EILs) in organic light-emitting devices (OLEDs). Four kinds of tetraalkylammonium hydroxides having different alkyl lengths were utilized as the exfoliation agents of a layered compound precursor HCa2Nb3O10 to synthesize CNO nanosheets, including tetramethylammonium hydroxide, tetraethylammonium hydroxide, tetrapropylammonium hydroxide (TPAOH), and tetrabutylammonium hydroxide. CNO nanosheet EILs were applied in fluorescent poly[(9,9-di- n-octylfluorenyl-2,7-diyl)- alt-(benzo[2,1,3]thiadiazol-4,8-diyl)] (F8BT) organic light-emitting polymer-based devices. The effects of dispersion concentrations and alkyl chain length on the devices' performances were investigated. The results demonstrated that OLEDs' performances were related to the coverage ratio of the CNO nanosheets, their thicknesses, and their work function values. Among the four exfoliation agents, the device with CNO nanosheets exfoliated by TPAOH showed the lowest driving voltage. The OLEDs with the CNO nanosheet EILs showed lower driving voltages compared with the devices with conventional EIL material lithium 8-quinolate.

16.
ACS Appl Mater Interfaces ; 10(29): 24607-24612, 2018 Jul 25.
Article in English | MEDLINE | ID: mdl-29968455

ABSTRACT

Cesium lead halide (CsPbX3, X = Cl, Br, or I) perovskite quantum dots (QDs) are known as ionic nanocrystals, and their optical properties are greatly affected by the washing solvent used during the purification process. Here, we demonstrate the purification process of CsPbBr3 perovskite QDs using low-dielectric-constant solvents to completely remove impurities, such as the reaction solvent and desorbed ligands. The use of the ether solvent diethylene glycol dimethyl ether (diglyme), having a low dielectric constant of ε = 7.23, as a poor solvent for reprecipitation allowed for multiple wash cycles, which led to high purity and high photoluminescence quantum yield for CsPbBr3 QDs. The light-emitting device constructed with the CsPbBr3 QDs and washed twice with diglyme (two-wash) showed a low turn-on voltage of 2.7 V and a peak external quantum efficiency of over 8%. Thus, the purification of perovskite QDs with multiple wash cycles using a low-dielectric-constant solvent is an effective approach for enhancing not only the optical properties but also the efficiency of perovskite quantum dot light-emitting devices.

17.
ACS Appl Mater Interfaces ; 10(20): 17318-17326, 2018 May 23.
Article in English | MEDLINE | ID: mdl-29714996

ABSTRACT

Electron injection layers (EILs) based on a simple polymer blend of polyethyleneimine ethoxylated (PEIE) and poly[(9,9-bis(3'-(( N, N-dimethyl)- N-ethylammonium)-propyl)-2,7-fluorene)- alt-2,7-(9,9-dioctylfluorene)] (PFN-Br) can suppress the dependence of organic light-emitting device (OLED) performance on thickness variation compared with single PEIE or PFN-Br EILs. PEIE and PFN-Br were compatible with each other and PFN-Br uniformly mixed in the PEIE matrix. PFN-Br in PEIE formed more fluorene-fluorene pairs than PFN-Br alone. In addition, PEIE:PFN-Br blends reduced the work function (WF) substantially compared with single PEIE or PFN-Br polymer. PEIE:PFN-Br blends were applied to EILs in fluorescent polymer-based OLEDs. Optimized PEIE:PFN-Br blend EIL-based devices presented lower driving voltages and smaller dependences of device performance on EIL thickness than single PEIE or PFN-Br-based devices. These improvements were attributed to electron-transporting fluorene moieties, increased fluorene-fluorene pairs working as channels of electron transport, and the large WF reduction effect of PEIE:PFN-Br blends.

18.
Adv Mater ; 30(18): e1705915, 2018 May.
Article in English | MEDLINE | ID: mdl-29532962

ABSTRACT

A lot of research, mostly using electron-injection layers (EILs) composed of alkali-metal compounds has been reported with a view to increase the efficiency of solution-processed organic light-emitting devices (OLEDs). However, these materials have intractable properties, such as a strong affinity for moisture, which cause the degradation of OLEDs. Consequently, optimal EIL materials should exhibit high electron-injection efficiency as well as be stable in air. In this study, polymer light-emitting devices (PLEDs) based on the commonly used yellow-fluorescence-emitting polymer F8BT, which utilize poly(diallyldimethylammonium)-based polymeric ionic liquids, are experimentally and analytically investigated. As a result, the optimized PLED employing an EIL comprising poly(diallyldimethylammonium) bis(trifluoromethanesulfonyl)imide (poly(DDA)TFSI), which is expected to display good moisture resistance because of water repellency of fluorocarbon groups, exhibits excellent storage stability in air and electroluminescence performance with a low turn-on voltage of 2.01 V, maximum external quantum efficiency of 9.00%, current efficiency of 30.1 cd A-1 , and power efficiency of 32.4 lm W-1 . The devices with poly(DDA)TFSI show one of the highest efficiencies as compared to the reported standard PLEDs. Moreover, poly(DDA)TFSI is applied as a hole-injection layer (HIL). The optimized PLED using poly(DDA)TFSI as the HIL exhibits performances comparable to those of a device that uses a conventional poly(3,4-ethylenedioxy-thiophene):poly(4-styrenesulfonate) HIL.

19.
Inorg Chem ; 57(4): 1950-1957, 2018 Feb 19.
Article in English | MEDLINE | ID: mdl-29420018

ABSTRACT

We report the development of solution-processed reduced phosphomolybdic acid (rPMA) containing molybdenum oxide units for post-treatment-free hole-injection layers (HILs) in organic light-emitting devices (OLEDs). The physical and chemical properties of rPMA, including its structure, solubility in several solvents, film surface roughness, work function, and valence states, were investigated. The formation of gap states just below the Fermi level of rPMA was observed. Without any post-treatment after the formation of rPMA films, OLEDs employing rPMA as an HIL exhibited a very low driving voltage and a high luminous efficiency. The low driving voltage was attributed to the energy level alignment between the gap states formed by reduction and the HOMO level of the hole-transport layer material N,N'-bis(1-naphthyl)-N,N'-diphenyl-(1,1'-biphenyl)-4,4'-diamine.

20.
ACS Appl Mater Interfaces ; 9(21): 18113-18119, 2017 May 31.
Article in English | MEDLINE | ID: mdl-28497949

ABSTRACT

Solution-processed electron injection layers (EILs) comprising lithium 8-quinolate (Liq) and polyethylenimine ethoxylated (PEIE) are highly effective for enhancing electron injection from ZnO to organic layers and improving device lifetime in organic light-emitting devices (OLEDs). Doping of Liq into PEIE further reduces the work function of zinc oxide (ZnO) by enhancing dipole formation. The intermolecular interaction between Liq and PEIE was elucidated by UV-vis absorption measurement and quantum chemical calculation. The OLEDs with ZnO covered with PEIE:Liq mixture exhibited lower driving voltage than that of the device without Liq. Furthermore, as doping concentration of Liq into PEIE increased, the device lifetime and voltage stability during constant current operation was successively improved.

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