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1.
Cell Mol Biol Lett ; 29(1): 39, 2024 Mar 19.
Artigo em Inglês | MEDLINE | ID: mdl-38504159

RESUMO

BACKGROUND: IGF2BP3 functions as an RNA-binding protein (RBP) and plays a role in the posttranscriptional control of mRNA localization, stability, and translation. Its dysregulation is frequently associated with tumorigenesis across various cancer types. Nonetheless, our understanding of how the expression of the IGF2BP3 gene is regulated remains limited. The specific functions and underlying mechanisms of IGF2BP3, as well as the potential benefits of targeting it for therapeutic purposes in bladder cancer, are not yet well comprehended. METHODS: The mRNA and protein expression were examined by RT-qPCR and western blotting, respectively. The methylation level of CpG sites was detected by Bisulfite sequencing PCR (BSP). The regulation of IGF2BP3 expression by miR-320a-3p was analyzed by luciferase reporter assay. The functional role of IGF2BP3 was determined through proliferation, colony formation, wound healing, invasion assays, and xenograft mouse model. The regulation of HMGB1 by IGF2BP3 was investigated by RNA immunoprecipitation (RIP) and mRNA stability assays. RESULTS: We observed a significant elevation in IGF2BP3 levels within bladder cancer samples, correlating with more advanced stages and grades, as well as an unfavorable prognosis. Subsequent investigations revealed that the upregulation of IGF2BP3 expression is triggered by copy number gain/amplification and promoter hypomethylation in various tumor types, including bladder cancer. Furthermore, miR-320a-3p was identified as another negative regulator in bladder cancer. Functionally, the upregulation of IGF2BP3 expression exacerbated bladder cancer progression, including the proliferation, migration, and invasion of bladder cancer. Conversely, IGF2BP3 silencing produced the opposite effects. Moreover, IGF2BP3 expression positively correlated with inflammation and immune infiltration in bladder cancer. Mechanistically, IGF2BP3 enhanced mRNA stability and promoted the expression of HMGB1 by binding to its mRNA, which is a factor that promotes inflammation and orchestrates tumorigenesis in many cancers. Importantly, pharmacological inhibition of HMGB1 with glycyrrhizin, a specific HMGB1 inhibitor, effectively reversed the cancer-promoting effects of IGF2BP3 overexpression in bladder cancer. Furthermore, the relationship between HMGB1 mRNA and IGF2PB3 is also observed in mammalian embryonic development, with the expression of both genes gradually decreasing as embryonic development progresses. CONCLUSIONS: Our present study sheds light on the genetic and epigenetic mechanisms governing IGF2BP3 expression, underscoring the critical involvement of the IGF2BP3-HMGB1 axis in driving bladder cancer progression. Additionally, it advocates for the investigation of inhibiting IGF2BP3-HMGB1 as a viable therapeutic approach for treating bladder cancer.


Assuntos
Proteína HMGB1 , MicroRNAs , Neoplasias da Bexiga Urinária , Humanos , Animais , Camundongos , MicroRNAs/genética , Proteína HMGB1/genética , Proteína HMGB1/metabolismo , Linhagem Celular Tumoral , Carcinogênese/genética , Metilação de DNA , Neoplasias da Bexiga Urinária/genética , Neoplasias da Bexiga Urinária/metabolismo , RNA Mensageiro/genética , RNA Mensageiro/metabolismo , Estabilidade de RNA , Inflamação/genética , Proliferação de Células/genética , Regulação Neoplásica da Expressão Gênica , Mamíferos/genética
2.
Food Chem ; 438: 138009, 2024 Apr 16.
Artigo em Inglês | MEDLINE | ID: mdl-37983991

RESUMO

In this work, a nontoxic crosslinking agent, citric acid (CA), was used to crosslink glycerol-plasticized SSPS films via a heat activated reaction. Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy results confirmed the occurrence of esterification reaction between CA and SSPS. Microstructure of the CA-crosslinked SSPS films were characterized by scanning electron microscopy, atomic force microscopy and X-ray diffraction. The water resistance, mechanical, UV-barrier, water vapor barrier, antioxidant and thermal properties of SSPS films were enhanced by CA crosslinking. The SSPS film crosslinked with 5 % CA exhibited a maximum tensile strength of 6.5 MPa and a minimum water solubility of 34.3 %. The CA-crosslinked SSPS film also presented superior antibacterial properties against Gram-positive and Gram-negative bacteria. Application test results showed that the CA-crosslinked SSPS film can effectively delay the oxidative deterioration of lard during storage, suggesting that the developed CA-crosslinked SSPS film could be a promising candidate for active food packaging.


Assuntos
Antibacterianos , Glycine max , Antibacterianos/farmacologia , Antibacterianos/química , Embalagem de Alimentos/métodos , Bactérias Gram-Negativas , Bactérias Gram-Positivas , Polissacarídeos/química , Permeabilidade
3.
J Phys Chem Lett ; 14(23): 5466-5474, 2023 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-37288806

RESUMO

Perovskite quantum dots (QDs) with high room-temperature luminescence efficiency have been applied in single-photon sources. While the optical properties of large, weakly confined perovskite nanocrystals have been extensively explored at the single-particle level, few studies have focused on single-perovskite QDs with strong quantum confinement. This is mainly due to their poor surface chemical stability. Here we demonstrate that strongly confined CsPbBr3 perovskite QDs (SCPQDs) embedded in a phenethylammonium bromide matrix exhibit a well-passivated surface and improved photostability under intense photoexcitation. We find that in our SCPQDs, photoluminescence blinking is suppressed at moderate excitation intensities, and increasing the excitation rates leads to weak photoluminescence intensity fluctuations accompanied by an unusual spectral blue-shift. We attribute this to a biexciton-like Auger interaction between excitons and trapped excitons formed by surface lattice elastic distortions. This hypothesis is corroborated by the unique repulsive biexciton interaction observed in the SCPQDs.

4.
Artigo em Inglês | MEDLINE | ID: mdl-36498120

RESUMO

Recently, global climate change has led to a high incidence of extreme weather and natural disasters. How to reduce its impact has become an important topic. However, the studies that both consider the disaster's real-time geographic information and environmental factors in severe rainstorms are still not enough. Volunteered geographic information (VGI) data that was generated during disasters offered possibilities for improving the emergency management abilities of decision-makers and the disaster self-rescue abilities of citizens. Through the case study of the extreme rainstorm disaster in Zhengzhou, China, in July 2021, this paper used machine learning to study VGI issued by residents. The vulnerable people and their demands were identified based on the SOS messages. The importance of various indicators was analyzed by combining open data from socio-economic and built-up environment elements. Potential safe areas with shelter resources in five administrative districts in the disaster-prone central area of Zhengzhou were identified based on these data. This study found that VGI can be a reliable data source for future disaster research. The characteristics of rainstorm hazards were concluded from the perspective of affected people and environmental indicators. The policy recommendations for disaster prevention in the context of public participation were also proposed.


Assuntos
Planejamento em Desastres , Desastres , Humanos , China , Mudança Climática
5.
J Am Chem Soc ; 144(45): 20923-20930, 2022 Nov 16.
Artigo em Inglês | MEDLINE | ID: mdl-36327099

RESUMO

InP-based quantum dot (QD) light-emitting diodes (QLEDs) provide a heavy-metal-free route to size-tuned LEDs having high efficiency. The stability of QLEDs may be enhanced by replacing organic hole-injection layers (HILs) with inorganic layers. However, inorganic HILs reported to date suffer from inefficient hole injection, the result of their shallow work functions. Here, we investigate the tuning of the work function of nickel oxide (NiOx) HILs using self-assembled molecules (SAMs). Density functional theory simulations and near-edge X-ray absorption fine structure put a particular focus onto the molecular orientation of the SAMs in tuning the work function of the NiOx HIL. We find that orientation plays an even stronger role than does the underlying molecular dipole itself: SAMs having the strongest electron-withdrawing nitro group (NO2), despite having a high intrinsic dipole, show limited work function tuning, something we assign to their orientation parallel to the NiOx surface. We further find that the NO2 group─which delocalizes electrons over the molecule by resonance─induces a deep lowest unoccupied molecular orbital level that accepts electrons from QDs, producing luminescence quenching. In contrast, SAMs containing a trifluoromethyl group exhibit an angled orientation relative to the NiOx surface, better activating hole injection into the active layer without inducing luminescence quenching. We report an external quantum efficiency (EQE) of 18.8%─the highest EQE among inorganic HIL-based QLEDs (including Cd-based QDs)─in InP QLEDs employing inorganic HILs.

6.
Int J Biol Macromol ; 222(Pt B): 3155-3167, 2022 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-36243153

RESUMO

Herein, a strong and stable gelatin-based composite hydrogel was fabricated by incorporation of amino-functionalized microfibrillated cellulose (AMFC) into gelatin matrix along with genipin crosslinking. The hydrogel consists of chemical and physical crosslinks among gelatin chains and AMFC fibrils. The morphology, swelling behavior and compressive properties of the composite hydrogels were investigated. The results show that the mechanical properties and structural stability of the gelatin hydrogels were improved remarkably by the addition of AMFC due to the formation of a hybrid network structure. The composite hydrogel has a compressive strength up to 1.52 MPa at a strain of 80 %, which is 41.2 and 1.8 times higher than that of the conventional physical and genipin-crosslinked gelatin hydrogels, respectively. Moreover, the developed gelatin-based composite hydrogels reinforced with AMFC exhibit good enzymatic stability, high surface hydrophobicity, tunable swelling property and excellent biocompatibility, which are expected to have potential applications in biomedical and pharmaceutical fields.


Assuntos
Gelatina , Hidrogéis , Gelatina/química , Hidrogéis/química , Celulose/química , Iridoides
7.
Adv Sci (Weinh) ; 9(24): e2201807, 2022 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-35794429

RESUMO

Solution-processed quasi-2D perovskites contain multiple quantum wells with a broad width distribution. Inhomogeneity results in the charge funneling into the smallest bandgap components, which hinders deep-blue emission and accelerates Auger recombination. Here, a synthetic strategy applied to a range of quasi-2D perovskite systems is reported, that significantly narrows the quantum well dispersity. It is shown that the phase distribution in the perovskite film is significantly narrowed with controlled, simultaneous evaporation of solvent and antisolvent. Modulation of film formation kinetics of quasi-2D perovskite enables stable deep-blue electroluminescence with a peak emission wavelength of 466 nm and a narrow linewidth of 14 nm. Light emitting diodes using the perovskite film show a maximum luminance of 280 cd m-2 at an external quantum efficiency of 0.1%. This synthetic approach will serve in producing new materials widening the color gamut of next-generation displays.

8.
ACS Appl Mater Interfaces ; 14(15): 17691-17697, 2022 Apr 20.
Artigo em Inglês | MEDLINE | ID: mdl-35411769

RESUMO

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.

9.
Adv Mater ; 34(21): e2200854, 2022 May.
Artigo em Inglês | MEDLINE | ID: mdl-35297516

RESUMO

Instability in mixed-halide perovskites (MHPs) is a key issue limiting perovskite solar cells and light-emitting diodes (LEDs). One form of instability arises during the processing of MHP quantum dots using an antisolvent to precipitate and purify the dots forming surface traps that lead to decreased luminescence, compromised colloidal stability, and emission broadening. Here, the introduction of inorganic ligands in the antisolvents used in dot purification is reported in order to overcome this problem. MHPs that are colloidally stable for over 1 year at 25 °C and 40% humidity are demonstrated and films that are stable under 100 W cm-2 photoirradiation, 4× longer than the best previously reported MHPs, are reported. In LEDs, the materials enable an EQE of 24.4% (average 22.5 ± 1.3%) and narrow emission (full-width at half maximum of 30 nm). Sixfold-enhanced operating stability relative to the most stable prior red perovskite LEDs having external quantum efficiency >20% is reported.

10.
J Am Chem Soc ; 144(9): 4009-4016, 2022 Mar 09.
Artigo em Inglês | MEDLINE | ID: mdl-35192324

RESUMO

The epitaxial growth of a perovskite matrix on quantum dots (QDs) has enabled the emergence of efficient red light-emitting diodes (LEDs) because it unites efficient charge transport with strong surface passivation. However, the synthesis of wide-band gap (Eg) QD-in-matrix heterostructures has so far remained elusive in the case of sky-blue LEDs. Here, we developed CsPbBr3 QD-in-perovskite matrix solids that enable high luminescent efficiency and spectral stability with an optical Eg of over 2.6 eV. We screened alloy candidates that modulate the perovskite Eg and allow heteroepitaxy, seeking to implement lattice-matched type-I band alignment. Specifically, we introduced a CsPb1-xSrxBr3 matrix, in which alloying with Sr2+ increased the Eg of the perovskite and minimized lattice mismatch. We then developed an approach to passivation that would overcome the hygroscopic nature of Sr2+. We found that bis(4-fluorophenyl)phenylphosphine oxide strongly coordinates with Sr2+ and provides steric hindrance to block H2O, a finding obtained by combining molecular dynamics simulations with experimental results. The resulting QD-in-matrix solids exhibit enhanced air- and photo-stability with efficient charge transport from the matrix to the QDs. LEDs made from this material exhibit an external quantum efficiency of 13.8% and a brightness exceeding 6000 cd m-2.

11.
Nature ; 599(7886): 594-598, 2021 11.
Artigo em Inglês | MEDLINE | ID: mdl-34819678

RESUMO

Light-emitting diodes (LEDs) based on perovskite quantum dots have shown external quantum efficiencies (EQEs) of over 23% and narrowband emission, but suffer from limited operating stability1. Reduced-dimensional perovskites (RDPs) consisting of quantum wells (QWs) separated by organic intercalating cations show high exciton binding energies and have the potential to increase the stability and the photoluminescence quantum yield2,3. However, until now, RDP-based LEDs have exhibited lower EQEs and inferior colour purities4-6. We posit that the presence of variably confined QWs may contribute to non-radiative recombination losses and broadened emission. Here we report bright RDPs with a more monodispersed QW thickness distribution, achieved through the use of a bifunctional molecular additive that simultaneously controls the RDP polydispersity while passivating the perovskite QW surfaces. We synthesize a fluorinated triphenylphosphine oxide additive that hydrogen bonds with the organic cations, controlling their diffusion during RDP film deposition and suppressing the formation of low-thickness QWs. The phosphine oxide moiety passivates the perovskite grain boundaries via coordination bonding with unsaturated sites, which suppresses defect formation. This results in compact, smooth and uniform RDP thin films with narrowband emission and high photoluminescence quantum yield. This enables LEDs with an EQE of 25.6% with an average of 22.1 ±1.2% over 40 devices, and an operating half-life of two hours at an initial luminance of 7,200 candela per metre squared, indicating tenfold-enhanced operating stability relative to the best-known perovskite LEDs with an EQE exceeding 20%1,4-6.

12.
J Am Chem Soc ; 143(38): 15606-15615, 2021 Sep 29.
Artigo em Inglês | MEDLINE | ID: mdl-34542273

RESUMO

Light-emitting diodes (LEDs) based on metal halide perovskite quantum dots (QDs) have achieved impressive external quantum efficiencies; however, the lack of surface protection of QDs, combined with efficiency droop, decreases device operating lifetime at brightnesses of interest. The epitaxial incorporation of QDs within a semiconducting shell provides surface passivation and exciton confinement. Achieving this goal in the case of perovskite QDs remains an unsolved challenge in view of the materials' chemical instability. Here, we report perovskite QDs that remain stable in a thin layer of precursor solution of perovskite, and we use strained QDs as nucleation centers to drive the homogeneous crystallization of a perovskite matrix. Type-I band alignment ensures that the QDs are charge acceptors and radiative emitters. The new materials show suppressed Auger bi-excition recombination and bright luminescence at high excitation (600 W cm-2), whereas control materials exhibit severe bleaching. Primary red LEDs based on the new materials show an external quantum efficiency of 18%, and these retain high performance to brightnesses exceeding 4700 cd m-2. The new materials enable LEDs having an operating half-life of 2400 h at an initial luminance of 100 cd m-2, representing a 100-fold enhancement relative to the best primary red perovskite LEDs.

13.
Adv Mater ; 33(41): e2103394, 2021 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-34425038

RESUMO

The open-circuit voltage (Voc ) of perovskite solar cells is limited by non-radiative recombination at perovskite/carrier transport layer (CTL) interfaces. 2D perovskite post-treatments offer a means to passivate the top interface; whereas, accessing and passivating the buried interface underneath the perovskite film requires new material synthesis strategies. It is posited that perovskite ink containing species that bind strongly to substrates can spontaneously form a passivating layer with the bottom CTL. The concept using organic spacer cations with rich NH2 groups is implemented, where readily available hydrogens have large binding affinity to under-coordinated oxygens on the metal oxide substrate surface, inducing preferential crystallization of a thin 2D layer at the buried interface. The passivation effect of this 2D layer is examined using steady-state and time-resolved photoluminescence spectroscopy: the 2D interlayer suppresses non-radiative recombination at the buried perovskite/CTL interface, leading to a 72% reduction in surface recombination velocity. This strategy enables a 65 mV increase in Voc for NiOx based p-i-n devices, and a 100 mV increase in Voc for SnO2 -based n-i-p devices. Inverted solar cells with 20.1% power conversion efficiency (PCE) for 1.70 eV and 22.9% PCE for 1.55 eV bandgap perovskites are demonstrated.

14.
Angew Chem Int Ed Engl ; 60(29): 16164-16170, 2021 Jul 12.
Artigo em Inglês | MEDLINE | ID: mdl-33982380

RESUMO

The all-inorganic nature of CsPbI3 perovskites allows to enhance stability in perovskite devices. Research efforts have led to improved stability of the black phase in CsPbI3 films; however, these strategies-including strain and doping-are based on organic-ligand-capped perovskites, which prevent perovskites from forming the close-packed quantum dot (QD) solids necessary to achieve high charge and thermal transport. We developed an inorganic ligand exchange that leads to CsPbI3 QD films with superior phase stability and increased thermal transport. The atomic-ligand-exchanged QD films, once mechanically coupled, exhibit improved phase stability, and we link this to distributing strain across the film. Operando measurements of the temperature of the LEDs indicate that KI-exchanged QD films exhibit increased thermal transport compared to controls that rely on organic ligands. The LEDs exhibit a maximum EQE of 23 % with an electroluminescence emission centered at 640 nm (FWHM: ≈31 nm). These red LEDs provide an operating half-lifetime of 10 h (luminance of 200 cd m-2 ) and an operating stability that is 6× higher than that of control devices.

15.
Adv Mater ; 33(5): e2006697, 2021 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-33349998

RESUMO

Metal halide perovskites have emerged as promising candidates for solution-processed laser gain materials, with impressive performance in the green and red spectral regions. Despite exciting progress, deep-blue-an important wavelength for laser applications-remains underexplored; indeed, cavity integration and single-mode lasing from large-bandgap perovskites have yet to be achieved. Here, a vapor-assisted chlorination strategy that enables synthesis of low-dimensional CsPbCl3  thin films exhibiting deep-blue emission is reported. Using this approach,  high-quality perovskite thin films having a low surface roughness (RMS ≈ 1.3 nm) and efficient charge transfer properties are achieved. These enable us to document low-threshold amplified spontaneous emission. Levering the high quality of the gain medium,  vertical-cavity surface-emitting lasers with a low lasing threshold of 6.5 µJ cm-2  are fabricated. This report of deep-blue perovskite single-mode lasing showcases the prospect of increasing the range of deep-blue laser sources.

16.
Sci Adv ; 6(42)2020 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-33055155

RESUMO

It remains a central challenge to the information display community to develop red light-emitting diodes (LEDs) that meet demanding color coordinate requirements for wide color gamut displays. Here, we report high-efficiency, lead-free (PEA)2SnI4 perovskite LEDs (PeLEDs) with color coordinates (0.708, 0.292) that fulfill the Rec. 2100 specification for red emitters. Using valeric acid (VA)-which we show to be strongly coordinated to Sn2+-we slow the crystallization rate of the perovskite, improving the film morphology. The incorporation of VA also protects tin from undesired oxidation during the film-forming process. The improved films and the reduced Sn4+ content enable PeLEDs with an external quantum efficiency of 5% and an operating half-life exceeding 15 hours at an initial brightness of 20 cd/m2 This work illustrates the potential of Cd- and Pb-free PeLEDs for display technology.

17.
Nat Nanotechnol ; 15(8): 668-674, 2020 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-32632321

RESUMO

Colloidal quantum dot (QD) solids are emerging semiconductors that have been actively explored in fundamental studies of charge transport1 and for applications in optoelectronics2. Forming high-quality QD solids-necessary for device fabrication-requires substitution of the long organic ligands used for synthesis with short ligands that provide increased QD coupling and improved charge transport3. However, in perovskite QDs, the polar solvents used to carry out the ligand exchange decompose the highly ionic perovskites4. Here we report perovskite QD resurfacing to achieve a bipolar shell consisting of an inner anion shell, and an outer shell comprised of cations and polar solvent molecules. The outer shell is electrostatically adsorbed to the negatively charged inner shell. This approach produces strongly confined perovskite QD solids that feature improved carrier mobility (≥0.01 cm2 V-1 s-1) and reduced trap density relative to previously reported low-dimensional perovskites. Blue-emitting QD films exhibit photoluminescence quantum yields exceeding 90%. By exploiting the improved mobility, we have been able to fabricate CsPbBr3 QD-based efficient blue and green light-emitting diodes. Blue devices with reduced trap density have an external quantum efficiency of 12.3%; the green devices achieve an external quantum efficiency of 22%.

18.
Nat Commun ; 11(1): 3674, 2020 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-32699223

RESUMO

Metal halide perovskites have emerged as promising candidates for solution-processed blue light-emitting diodes (LEDs). However, halide phase segregation - and the resultant spectral shift - at LED operating voltages hinders their application. Here we report true-blue LEDs employing quasi-two-dimensional cesium lead bromide with a narrow size distribution of quantum wells, achieved through the incorporation of a chelating additive. Ultrafast transient absorption spectroscopy measurements reveal that the chelating agent helps to control the quantum well thickness distribution. Density functional theory calculations show that the chelating molecule destabilizes the lead species on the quantum well surface and that this in turn suppresses the growth of thicker quantum wells. Treatment with γ-aminobutyric acid passivates electronic traps and enables films to withstand 100 °C for 24 h without changes to their emission spectrum. LEDs incorporating γ-aminobutyric acid-treated perovskites exhibit blue emission with Commission Internationale de l'Éclairage coordinates of (0.12, 0.14) at an external quantum efficiency of 6.3%.

19.
Adv Sci (Weinh) ; 7(8): 1903213, 2020 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-32328423

RESUMO

Perovskite-based light-emitting diodes (PeLEDs) are now approaching the upper limits of external quantum efficiency (EQE); however, their application is currently limited by reliance on lead and by inadequate color purity. The Rec. 2020 requires Commission Internationale de l'Eclairage coordinates of (0.708, 0.292) for red emitters, but present-day perovskite devices only achieve (0.71, 0.28). Here, lead-free PeLEDs are reported with color coordinates of (0.706, 0.294)-the highest purity reported among red PeLEDs. The variation of the emission spectrum is also evaluated as a function of temperature and applied potential, finding that emission redshifts by <3 nm under low temperature and by <0.3 nm V-1 with operating voltage. The prominent oxidation pathway of Sn is identified and this is suppressed with the aid of H3PO2. This strategy prevents the oxidation of the constituent precursors, through both its moderate reducing properties and through its forming complexes with the perovskite that increase the energetic barrier toward Sn oxidation. The H3PO2 additionally seeds crystal growth during film formation, improving film quality. PeLEDs are reported with an EQE of 0.3% and a brightness of 70 cd m-2; this is the record among reported red-emitting, lead-free PeLEDs.

20.
Nano Lett ; 20(5): 3694-3702, 2020 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-32227970

RESUMO

Increasing the power conversion efficiency (PCE) of colloidal quantum dot (CQD) solar cells has relied on improving the passivation of CQD surfaces, enhancing CQD coupling and charge transport, and advancing device architecture. The presence of hydroxyl groups on the nanoparticle surface, as well as dimers-fusion between CQDs-has been found to be the major source of trap states, detrimental to optoelectronic properties and device performance. Here, we introduce a CQD reconstruction step that decreases surface hydroxyl groups and dimers simultaneously. We explored the dynamic interaction of charge carriers between band-edge states and trap states in CQDs using time-resolved spectroscopy, showing that trap to ground-state recombination occurs mainly from surface defects in coupled CQD solids passivated using simple metal halides. Using CQD reconstruction, we demonstrate a 60% reduction in trap density and a 25% improvement in charge diffusion length. These translate into a PCE of 12.5% compared to 10.9% for control CQDs.

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