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1.
ACS Nano ; 18(11): 8157-8167, 2024 Mar 19.
Article in English | MEDLINE | ID: mdl-38456777

ABSTRACT

Perovskite light-emitting diodes (PeLEDs) are the next promising display technologies because of their high color purity and wide color gamut, while two classical emitter forms, i.e., polycrystalline domains and quantum dots, are encountering bottlenecks. Weak carrier confinement of large polycrystalline domains leads to inadequate radiative recombination, and surface ligands on quantum dots are the main annihilation sites for injected carriers. Here, pinpointing these issues, we screened out an amphoteric agent, namely, 2-(2-aminobenzoyl)benzoic acid (2-BA), to precisely control the in situ growth of FAPbI3 (FA: formamidine) nanodomains with enhanced space confinement, preferred crystal orientation, and passivated trap states on the transport-layer substrate. The amphoteric 2-BA performs bidentate chelating functions on the formation of ultrasmall perovskite colloids (<1 nm) in the precursor, resulting in a smoother FAPbI3 emitting layer. Based on monodispersed and homogeneous nanodomain films, a near-infrared PeLED device with a champion efficiency of >22% plus enhanced T80 operational stability was achieved. The proposed perovskite nanodomain film tends to be a mainstream emitter toward the performance breakthrough of PeLED devices covering visible wavelengths beyond infrared.

2.
Nature ; 625(7995): 516-522, 2024 Jan.
Article in English | MEDLINE | ID: mdl-38233617

ABSTRACT

Perovskite solar cells (PSCs) comprise a solid perovskite absorber sandwiched between several layers of different charge-selective materials, ensuring unidirectional current flow and high voltage output of the devices1,2. A 'buffer material' between the electron-selective layer and the metal electrode in p-type/intrinsic/n-type (p-i-n) PSCs (also known as inverted PSCs) enables electrons to flow from the electron-selective layer to the electrode3-5. Furthermore, it acts as a barrier inhibiting the inter-diffusion of harmful species into or degradation products out of the perovskite absorber6-8. Thus far, evaporable organic molecules9,10 and atomic-layer-deposited metal oxides11,12 have been successful, but each has specific imperfections. Here we report a chemically stable and multifunctional buffer material, ytterbium oxide (YbOx), for p-i-n PSCs by scalable thermal evaporation deposition. We used this YbOx buffer in the p-i-n PSCs with a narrow-bandgap perovskite absorber, yielding a certified power conversion efficiency of more than 25%. We also demonstrate the broad applicability of YbOx in enabling highly efficient PSCs from various types of perovskite absorber layer, delivering state-of-the-art efficiencies of 20.1% for the wide-bandgap perovskite absorber and 22.1% for the mid-bandgap perovskite absorber, respectively. Moreover, when subjected to ISOS-L-3 accelerated ageing, encapsulated devices with YbOx exhibit markedly enhanced device stability.

3.
Adv Mater ; 36(2): e2305238, 2024 Jan.
Article in English | MEDLINE | ID: mdl-37665975

ABSTRACT

The limited conductivity of existing transparent conducting oxide (TCO) greatly restricts the further performance improvement of perovskite solar cells (PSCs), especially for large-area devices. Herein, buried-metal-grid tin-doped indium oxide (BMG ITO) electrodes are developed to minimize the power loss caused by the undesirable high sheet resistance of TCOs. By burying 140-nm-thick metal grids into ITO using a photolithography technique, the sheet resistance of ITO is reduced from 15.0 to 2.7 Ω sq-1 . The metal step of BMG over ITO has a huge impact on the charge carrier transport in PSCs. The PSCs using BMG ITO with a low metal step deliver power conversion efficiencies (PCEs) significantly better than that of their counterparts with higher metal steps. Moreover, compared with the pristine ITO-based PSCs, the BMG ITO-based PSCs show a smaller PCE decrease when scaling up the active area of devices. The parallel-connected large-area PSCs with an active area of 102.8 mm2 reach a PCE of 22.5%. The BMG ITO electrodes are also compatible with the fabrication of inverted-structure PSCs and organic solar cells. The work demonstrates the great efficacy of improving the conductivity of TCO by BMG and opens up a promising avenue for constructing highly efficient large-area PSCs.

4.
Sci Total Environ ; 868: 161755, 2023 Apr 10.
Article in English | MEDLINE | ID: mdl-36690099

ABSTRACT

The extreme change of water storage in the Yangtze River Basin (YRB) have a significant impact on identifying the characteristics of drought events in the basin. To quantify the historical hydrological drought characteristics, we put forward new framework to reconstruct the pre-2003 total water storage anomaly (TWSA) through the nonlinear autoregressive with exogenous input (NARX) model. The NARX model is developed by the Gravity Recovery and Climate Experiment (GRACE) based TWSA and the hydrometeorological data after removing the trend and seasonal signals from 2003 to 2017, then the full pre-2003 reconstructed TWSA signals were obtained by synthesizing hydrometeorological data driven NARX model results from 1979 to 2002 and GRACE-estimated seasonal cycle. We combined the reconstructed TWSA with GRACE observed TWSA to characterize the historical hydrological drought events (onset, end, duration, magnitude, intensity, and recovery) in the YRB. The results show that the drought-related extreme anomalies in total water storage can be captured successfully. From 1979 to 2017, 23 hydrological drought events were identified in the YRB with an average recovery time of 4.7 months. The longest drought lasted 28 months spanning from July 2006 to October 2008. The exceptional drought occurred in September 2011 reached to the largest deficit with a magnitude of -48.5 mm and minimum drought severity index (DSI) of -2.3. Comparing to the period of 1979-1999, the frequency, duration, and average recovery time of drought events increased significantly since 2000 in the YRB. Furthermore, we found that the duration and average recovery time of the drought events have an exponential relationship with the severity, which could help us to estimate the potential recovery time when drought events occur and predict water resources dynamic in the future.

5.
World J Gastroenterol ; 28(45): 6363-6379, 2022 Dec 07.
Article in English | MEDLINE | ID: mdl-36533112

ABSTRACT

Gastrointestinal (GI) cancers are the major cause of cancer-related mortality globally. Medical imaging is an important auxiliary means for the diagnosis, assessment and prognostic prediction of GI cancers. Radiomics is an emerging and effective technology to decipher the encoded information within medical images, and traditional machine learning is the most commonly used tool. Recent advances in deep learning technology have further promoted the development of radiomics. In the field of GI cancer, although there are several surveys on radiomics, there is no specific review on the application of deep-learning-based radiomics (DLR). In this review, a search was conducted on Web of Science, PubMed, and Google Scholar with an emphasis on the application of DLR for GI cancers, including esophageal, gastric, liver, pancreatic, and colorectal cancers. Besides, the challenges and recommendations based on the findings of the review are comprehensively analyzed to advance DLR.


Subject(s)
Deep Learning , Gastrointestinal Neoplasms , Humans , Prognosis , Machine Learning , Diagnostic Imaging/methods , Gastrointestinal Neoplasms/diagnostic imaging , Gastrointestinal Neoplasms/therapy
6.
ACS Appl Mater Interfaces ; 12(33): 37774-37783, 2020 Aug 19.
Article in English | MEDLINE | ID: mdl-32814399

ABSTRACT

Shape-engineered nanocrystals (SENs) promise a better selectivity and a higher activity in catalytic reactions than the corresponding non-shape-engineered ones because of their larger specific surface areas and desirable crystal facets. However, often, it is challenging to apply SENs in practical catalytic applications at high reaction temperatures, where SENs deforms into more stable, less active nanoparticles. In this paper, we show that atomic layer deposition (ALD) of Al2O3 at 200 °C can controllably dope Al cations into the shape-engineered CeO2 nanorods (NRs) to not only increase their shape transition temperature from 400 °C to beyond 700 °C but also greatly increase their specific reversible oxygen storage capacity (srOSC). The substituted Al3+ ions impede the surface diffusion of Ce ions and therefore improve the thermal stability of CeO2 NRs. These Al3+ dopants form -Al-O-Ce-O- clusters, which are new Ce species and can be reversibly reduced and oxidized at 500-700 °C. This low-temperature chemical doping method decouples the synthesis process of SENs from the doping process and maintains the shape of the SENs during the activation of dopants. This concept could be adopted to enable the applications of other SENs in challenging high-temperature environments.

7.
Langmuir ; 35(20): 6522-6531, 2019 May 21.
Article in English | MEDLINE | ID: mdl-31035746

ABSTRACT

Al2O3 atomic layer deposition (ALD), which uses trimethylaluminum (TMA) as the metal precursor, shows promise in improving the environmental stability of hybrid halide perovskites. However, it is not yet entirely clear how TMA, a strong Lewis acid, reacts with fresh perovskites and how the reaction affects the nucleation of ALD Al2O3. Here, the effects of reaction temperature and partial pressure of TMA on the mechanisms of TMA/CH3NH3PbI3 reactions are investigated. Our real time mass gain data and in situ mass spectrometry data show that the TMA/CH3NH3PbI3 reaction can either remove mass or accumulate mass onto CH3NH3PbI3 substrates, depending strongly on the reaction temperature and partial pressure of TMA. The TMA/CH3NH3PbI3 reaction probably generates TMA-CH3NHx adduct compounds, which protects CH3NH3PbI3 from TMA by forming a shell at 25 °C in the vacuum process. However, these adduct compounds decompose at higher temperatures (e.g., 75 °C). This product layer is much thicker than a monolayer, suggesting the interface formed between Al2O3 coating and CH3NH3PbI3 is blurring and messy. These results have not yet, but should be, carefully considered to correctly interpret the effect of ALD Al2O3 treatment on optoelectronic properties of CH3NH3PbI3.

8.
ACS Appl Mater Interfaces ; 11(22): 20453-20464, 2019 Jun 05.
Article in English | MEDLINE | ID: mdl-31095374

ABSTRACT

Wearable strain sensors are essential for the realization of applications in the broad fields of remote healthcare monitoring, soft robots, and immersive gaming, among many others. These flexible sensors should be comfortably adhered to the skin and capable of monitoring human motions with high accuracy, as well as exhibiting excellent durability. However, it is challenging to develop electronic materials that possess the properties of skin-compliant, elastic, stretchable, and self-healable. This work demonstrates a new regenerative polymer complex composed of poly(2-acrylamido-2-methyl-1-propanesulfonic acid), polyaniline, and phytic acid as a skin-like electronic material. It exhibits ultrahigh stretchability (1935%), repeatable autonomous self-healing ability (repeating healing efficiency >98%), quadratic response to strain ( R2 > 0.9998), and linear response to flexion bending ( R2 > 0.9994), outperforming current reported wearable strain sensors. The deprotonated polyelectrolyte, multivalent anion, and doped conductive polymer, under ambient conditions, synergistically construct a regenerative dynamic network of polymer complex cross-linked by hydrogen bonds and electrostatic interactions, which enables ultrahigh stretchability and repeatable self-healing. Sensitive strain-responsive geometric and piezoresistive mechanisms of the material owing to the homogeneous and viscoelastic nature provide excellent linear responses to omnidirectional tensile strain and bending deformations. Furthermore, this material is scalable and simple to process in an environmentally friendly manner, paving the way for the next-generation flexible electronics.

9.
ACS Appl Mater Interfaces ; 10(34): 28948-28954, 2018 Aug 29.
Article in English | MEDLINE | ID: mdl-30058323

ABSTRACT

Atomic layer deposition (ALD) of oxide film on [6,6]-phenyl-C61 butyric acid methyl ester (PCBM) shows a great promise to dramatically improve the ambient stability of hybrid halide perovskite. The nucleation of an ALD oxide on PCBM is critical to reliably apply this strategy. In this paper, we present the first study of the nucleation behavior of ALD oxides, including Al2O3 and ZnO, on PCBM. We find that PCBM film acts a gas diffusion barrier blocking the ALD reactants (diethyl zinc) from etching the underlying CH3NH3PbI3. However, ZnO is not able to nucleate on PCBM. We further identify that trimethyl aluminum, a strongly Lewis acid, reacts readily with C═O on PCBM to generate a seeding layer for nucleating ZnO ALD. This new chemical route is highly reliable and can be used to synthesize ALD ZnO coatings over PCBM. The synthesized PCBM/Al2O3-ZnO dramatically improves the stability of CH3NH3PbI3 against the ambience and even against liquid water. The result signifies the importance of understanding of nucleation of ALD in enabling reliable barrier coatings for hybrid halide perovskites.

10.
J Phys Chem A ; 121(36): 6755-6765, 2017 Sep 14.
Article in English | MEDLINE | ID: mdl-28806510

ABSTRACT

Pyridine molecules have been used to passivate surface Pb2+ sites of CH3NH3PbI3, to recrystallize CH3NH3PbI3, and to bleach CH3NH3PbI3. However, these results contradict each other, as recrystallization and optical-bleach require transformation of bulk CH3NH3PbI3, but surface passivation demands the confinement of the reaction at the surface region. The underlying mechanism for these seemly contradicting results is not yet understood. In this paper, we show, at 25 °C, partial pressure of pyridine vapor is a determining factor for its reaction behaviors with CH3NH3PbI3: one can modify the surface region of CH3NH3PbI3 by using pyridine vapor of pressure 1.15 torr or lower but can transform the whole bulk CH3NH3PbI3 film with a pyridine vapor of 1.3 torr or higher. Our result is the first demonstration that the reaction modes, i.e., surface-confined reaction and bulk transformation, are very sensitive to the partial pressure of under-saturated pyridine vapor. Despite the different reaction behaviors, it is interesting that in all pressure ranges, pyridinium ion is a main product from the reaction between pyridine and CH3NH3PbI3. The bulk transformation is due to the formation of a liquid-like film, which increases the mobility of species to catalyze the reaction between pyridine and CH3NH3PbI3. It is important to note 1.3 torr is much smaller than the saturated vapor pressure of pyridine (20 torr at 25 °C). These findings provide a guidance in applying pyridine and other amines to functionalize and transform CH3NH3PbI3 and other hybrid halide perovskites. It also highlights the critical role of fundamental studies in controllably modifying CH3NH3PbI3.

11.
Nanoscale ; 7(28): 11915-21, 2015 Jul 28.
Article in English | MEDLINE | ID: mdl-26118367

ABSTRACT

Bismuth telluride (Bi2Te3) two-dimensional (2D) nanosheets prepared by van der Waals epitaxy were successfully detached, transferred, and suspended for nano-indentation measurements to be performed on freestanding circular nanosheets. The Young's modulus acquired by fitting linear elastic behaviors of 26 samples (thickness: 5-14 nm) is only 11.7-25.7 GPa, significantly smaller than the bulk in-plane Young's modulus (50-55 GPa). Compliant and robust Bi2Te3 2D nanosheets suggest the feasibility of the elastic strain engineering of topological surface states.

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