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1.
J Am Chem Soc ; 144(18): 8162-8170, 2022 May 11.
Artículo en Inglés | MEDLINE | ID: mdl-35442667

RESUMEN

All-inorganic CsPbI3 perovskite is attractive for deep-red light-emitting diodes (LEDs) because of its excellent carrier mobility, high color purity, and solution processability. However, the high phase transition energy barrier of optically active CsPbI3 black phase hinders the fabrication of efficient and bright LEDs. Here, we report a novel α-BaF2 nanoparticle substrate-promoted solution-processable heteroepitaxial growth to overcome this hindrance and obtain high-quality optically active γ-CsPbI3 thin films, achieving efficient and bright deep-red LEDs. We unravel that the highly exposed planes on the α-BaF2 nanoparticle-based heteroepitaxial growth substrate have a 99.5% lattice matching degree with the (110) planes of γ-CsPbI3. This ultrahigh lattice matching degree initiates solution-processed interfacial strain-free epitaxial growth of low-defect and highly oriented γ-CsPbI3 thin films on the substrate. The obtained γ-CsPbI3 thin films are uniform, smooth, and highly luminescent, based on which we fabricate efficient and bright deep-red LEDs with a high peak external quantum efficiency of 14.1% and a record luminance of 1325 cd m-2.

2.
Nano Lett ; 21(20): 8756-8763, 2021 Oct 27.
Artículo en Inglés | MEDLINE | ID: mdl-34637318

RESUMEN

Metal halide perovskites are promising semiconductors for next-generation light-emitting diodes (LEDs) due to their high luminance, excellent color purity, and handily tunable band gap. However, it remains a great challenge to develop perovskite LEDs (PeLEDs) with pure red emission at the wavelength of 630 nm. Herein, we report a spectrally stable and efficient pure red PeLED by employing sequential ligand post-treated CsPbI3 quantum dots (QDs). The synthesized CsPbI3 QDs with a size of ∼5 nm are treated in sequential steps using the ligands of 1-hydroxy-3-phenylpropan-2-aminium iodide (HPAI) and tributylsulfonium iodide (TBSI), respectively. The CsPbI3 QD films exhibit improved optoelectronic properties, which enables the fabrication of a pure red PeLED with a peak external quantum efficiency (EQE) of 6.4% and a stable EL emission centered at the wavelength of 630 nm. Our reported sequential ligand post-treatment strategy opens a new route to improve the stability and efficiency of PeLEDs based on QDs.

3.
Angew Chem Int Ed Engl ; 61(38): e202208960, 2022 Sep 19.
Artículo en Inglés | MEDLINE | ID: mdl-35861476

RESUMEN

Thermochromic phosphors are intriguing materials for realizing thermochromic behaviors of light-emitting diodes. Here a highly luminescent and stable thermochromic phosphor based on one-dimensional Cu4 I6 (4-dimethylamino-1-ethylpyridinium)2 is reported. This unique ionic copper-iodine chain-based hybrid exhibits near-unity photoluminescence efficiency owing to the through-space charge-transfer character of relevant electronic transitions. More importantly, an alternative mechanism of thermochromic phosphorescence was unraveled, supported by a first principles simulation of concerted copper atom migration in the copper-iodine chain. Furthermore, we successfully fabricate a bright thermochromic light-emitting diode using this Cu4 I6 (4-dimethylamino-1-ethylpyridinium)2 thermochromic phosphor. Our reported flexible ionic copper-iodine chain-based thermochromic luminescent material represents a new type of cost-effective functional phosphor.

4.
J Am Chem Soc ; 143(47): 19928-19937, 2021 Dec 01.
Artículo en Inglés | MEDLINE | ID: mdl-34766754

RESUMEN

Lead halide perovskite nanocrystals (PNCs) are emerging as promising light emitters to be actively explored for high color purity and efficient light-emitting diodes. However, the most reported lead halide perovskite nanocrystal light-emitting diodes (PNCLEDs) encountered issues of emission line width broadening and operation voltage elevating caused by the quantum confinement effect. Here, we report a new type of PNCLED using large-size CsPbBr3 PNCs overly exceeding the Bohr exciton diameter, achieving ultranarrow emission line width and rapid brightness rise around the turn-on voltage. We adopt calcium-tributylphosphine oxide hybrid ligand passivation to produce highly dispersed large-size colloidal CsPbBr3 PNCs with a weak size confinement effect and also high photoluminescence quantum yield (∼85%). Utilizing these large-size PNCs as emitters, we manifest that the detrimental effects caused by the quantum confinement effect can be avoided in the device, thereby realizing the highest color purity in green PNCLED, with a narrow full width at half-maximum of 16.4 nm and a high corrected maximum external quantum efficiency of 17.85%. Moreover, the operation half-life time of the large-size PNCLED is 5-fold of that based on smaller-size PNCs. Our work provides a new avenue for improving the performance of PNCLEDs based on unconventional large-size effects.

5.
J Am Chem Soc ; 142(6): 2956-2967, 2020 Feb 12.
Artículo en Inglés | MEDLINE | ID: mdl-31902206

RESUMEN

All-inorganic lead halide perovskite nanocrystals (NCs) are potential candidates for fabricating high-performance light-emitting diodes (LEDs) owing to their precisely tunable bandgaps, high photoluminescence (PL) efficiency, and excellent color purities. However, the performance of pure red (630-640 nm) all-inorganic perovskite LEDs is still limited by the halide segregation-induced instability of the electroluminescence (EL) of mixed halide CsPbI3-xBrx NCs. Herein, we report an effective approach to improving the EL stability of pure red all-inorganic CsPbI3-xBrx NC-based LEDs via the passivation of potassium bromide on NCs. By adding potassium oleate to the reaction system, we obtained potassium bromide surface-passivated (KBr-passivated) CsPbI3-xBrx NCs with pure red PL emission and a photoluminescence quantum yield (PLQY) exceeding 90%. We determine that most potassium ions present on the surface of NCs bind with bromide ions and thus demonstrate that potassium bromide surface passivation of NCs can both improve the PL stability and inhibit the halide segregation of NCs. Using KBr-passivated CsPbI3-xBrx NCs as an emitting layer, we fabricated stable and pure red perovskite LEDs with emission at 637 nm, showing a maximum brightness of 2671 cd m-2, maximum external quantum efficiency of 3.55%, and good EL stability. The proposed KBr-passivated NC strategy will open a new avenue for fabricating efficient, stable, and tunable pure color perovskite NC LEDs.

6.
Immun Inflamm Dis ; 11(7): e911, 2023 07.
Artículo en Inglés | MEDLINE | ID: mdl-37506134

RESUMEN

OBJECTIVE: To investigate DNA methylation (DNAm) status of dickkopf-associated protein 1 (DKK-1) in ossified hip capsule synovium and serum among patients with ankylosing spondylitis (AS). METHODS: Western blot was applied to detect the level of DKK-1 protein expression in hip joint capsule tissues from four patients with AS as well as four patients with femoral neck fracture (FNF) caused by trauma as control. DKK-1 gene promoter methylation (GPM) was examined by methylation-specific polymerase chain reaction. Reverse transcription-polymerase chain reaction was performed to examine the messenger RNA (mRNA) levels of DKK-1, ß-catenin, and Wnt3a in both tissue and serum. The DNAm status of serum DKK-1 was measured among 36 patients with AS and syndesmophytes (AS + syndesmophytes group), 40 patients with AS but no syndesmophyte (AS group), and 42 healthy individuals (control group). Also, the serum levels of DKK-1 were measured by enzyme-linked immunosorbent assay. The modified New York criteria (mNYC) together with the modified Stoke Ankylosing Spondylitis Spinal Score (mSASSS) were adopted to examine the radiographic progression of AS. The receiver operating characteristic (ROC) curve was applied to investigate the diagnostic value of the methylation rate of DKK-1 with regard to radiographic progression. RESULTS: The expressions of DKK-1 protein and mRNA in hip joint capsule tissues of AS patients were significantly lower, while DKK-1 GPM rate, ß-catenin mRNA, and Wnt3a mRNA were markedly higher when compared with FNF group. For serum samples, the DKK-1 methylation rate was significantly higher in AS+ syndesmophytes group in contrast to AS group and healthy controls. Serum levels of DKK-1 protein and mRNA in AS with syndesmophytes group were markedly decreased, while ß-catenin mRNA and Wnt3a mRNA expressions were significantly increased than AS with no syndesmophyte group and the healthy control group. AS patients in Grade 4 showed a significantly higher serum DKK-1 GPM rate than those in Grade 3 based on mNYC. Serum DKK-1 GPM level was markedly and positively correlated with mSASSS. Serum levels of DKK-1 in AS+ syndesmophytes group were markedly lower compared with AS but no syndesmophyte group and healthy controls. ROC curve analysis indicated that serum DKK-1 methylation rate serves as a decent indicator for AS radiographic progression. CONCLUSION: DNAm of DKK-1 may correlate with pathological bone formation in AS, which may provide new strategies for the treatment of AS abnormal bone formation.


Asunto(s)
Espondilitis Anquilosante , Humanos , beta Catenina/genética , Metilación de ADN , Osteogénesis , Columna Vertebral/patología , Espondilitis Anquilosante/genética
7.
Sci Adv ; 8(45): eabq2321, 2022 Nov 11.
Artículo en Inglés | MEDLINE | ID: mdl-36367940

RESUMEN

Solution-processable all-inorganic CsPbI3-xBrx perovskite holds great potential for pure red light-emitting diodes. However, the widely existing defects in this mixed halide perovskite markedly limit the efficiency and stability of present light-emitting diode devices. We here identify that intragrain Ruddlesden-Popper planar defects are primary forms of such defects in the CsPbI3-xBrx thin film owing to the lattice strain caused by inhomogeneous halogen ion distribution. To eliminate these defects, we develop a stepwise metastable phase crystallization strategy to minimize the CsPbI3-xBrx perovskite lattice strain, which brings planar defect-free CsPbI3-xBrx thin film with improved radiative recombination, narrowed emission band, and enhanced spectral stability. Using these high-quality thin films, we fabricate spectrally stable pure red perovskite light-emitting diodes, showing 17.8% external quantum efficiency and 9000 candela meter-2 brightness with color coordinates required by Rec. 2020.

8.
J Phys Chem Lett ; 11(21): 9371-9378, 2020 Nov 05.
Artículo en Inglés | MEDLINE | ID: mdl-33095581

RESUMEN

All-inorganic cesium lead halide perovskite colloidal nanocrystals are attractive for next-generation light-emitting diodes because of their high color purity, but the nonradiative Auger recombination in perovskite nanocrystal film limits the efficiency and brightness of the fabricated devices. Here, we introduce a surface-engineering process to exchange the original long-chain oleic acid/oleylamine ligands by the cerium-tributylphosphine oxide hybrid ligands to suppress nonradiative Auger recombination in CsPbBr3 NC film for bright and low-efficiency roll-off light-emitting diodes. Using ultrafast transient absorption and time-resolved photoluminescence spectroscopy, we demonstrate that the hybrid ligand passivation can efficiently remove surface trap states to enhance radiative recombination and homogenize the exciton concentration to suppress nonradiative Auger recombination in the CsPbBr3 nanocrystal thin film. Consequently, we fabricate a light-emitting diode with efficient charge injection into the CsPbBr3 nanocrystal emitting layer, achieving a pronounced improvement of electroluminescence with an external quantum efficiency from 5.5% to 9.1%. More importantly, the efficiency roll-off characteristics of high-brightness light-emitting diodes is effectively mitigated. Our reported hybrid ligand passivation suppressed Auger recombination strategy shows a great potential for fabricating high-brightness cesium lead halide perovskite light-emitting diodes.

9.
Transcult Psychiatry ; 55(3): 317-338, 2018 06.
Artículo en Inglés | MEDLINE | ID: mdl-29553307

RESUMEN

Bipolar disorder (BD) affects a significant proportion of Taiwanese individuals (Weissman et al., 1996; Yang, Yeh, & Hwu, 2012). Psychotropic medications are typically the mainstay of treatment for BD, and there is an abundance of international research on biological etiology and medication options. However, there is comparatively little research on psychosocial aspects of BD, including how it is understood and managed within families. As culture provides the context in which psychiatric disease is managed, there is a need to identify distinct Chinese psychosocial perspectives that might shed light on intervention options. This research explored how Taiwanese patients and family members comprehend and cope with BD. A sample of 42 participants, including 20 Taiwanese patients diagnosed with Bipolar Disorder-I (BD-I) for at least 4 years, and 22 family members, participated in separate interviews on explanatory models of illness. Qualitative thematic analysis focused on features that were distinct from those in current Western research literature. Five themes were identified that represented Taiwanese conceptualizations of BD, notions of etiology, views regarding treatment, and the difficulties in managing the disorder. Participants used Chinese language terms and descriptions of BD that reflected greater concerns about irritability, anger, and family conflict than about other symptoms, and participants also emphasized characterological trait descriptions of the condition. Their responses reflected their acceptance of lifelong family responsibility for caretaking, clashing beliefs regarding biomedical versus traditional Chinese medical and spiritual models of etiology and cure, profound concerns about the effects of psychiatric medication on the liver and kidney systems, and a focus on stress rather than genetic or biological models of etiology.


Asunto(s)
Trastorno Bipolar/etnología , Trastorno Bipolar/terapia , Familia/etnología , Conocimientos, Actitudes y Práctica en Salud/etnología , Adulto , Femenino , Humanos , Masculino , Persona de Mediana Edad , Taiwán/etnología , Adulto Joven
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