The two-dimensional (2D) perovskites stabilized by alternating cations in the interlayer space (ACI) define a new type of structure with different physical properties than the more common Ruddlesden−Popper counterparts. However, there is a lack of understanding of material crystallization in films and its influence on the morphological/optoelectronic properties and the final photovoltaic devices. Herein, we undertake in situ studies of the solidification process for ACI 2D perovskite (GA)(MA) n Pb n I 3n+1 (⟨n⟩ = 3) from ink to solid-state semiconductor, using solvent mixture of DMSO:DMF (1:10 v/v) as the solvent and link this behavior to solar cell devices. The in situ grazing-incidence X-ray scattering (GIWAXS) analysis reveals a complex journey through disordered sol−gel precursors, intermediate phases, and ultimately to ACI perovskites. The intermediate phases, including a crystalline solvate compound and the 2D GA 2 PbI 4 perovskite, provide a scaffold for the growth of the ACI perovskites during thermal annealing. We identify 2D GA 2 PbI 4 to be the key intermediate phase, which is strongly influenced by the deposition technique and determines the formation of the 1D GAPbI 3 byproducts and the distribution of various n phases of ACI perovskites in the final films. We also confirm the presence of internal charge transfer between different n phases through transient absorption spectroscopy. The high quality ACI perovskite films deposited from solvent mixture of DMSO:DMF (1:10 v/v) deliver a record power conversion efficiency of 14.7% in planar solar cells and significantly enhanced long-term stability of devices in contrast to the 3D MAPbI 3 counterpart.
Layered Ruddlesden–Popper (RP) phase (2D) halide perovskites have attracted tremendous attention due to the wide tunability on their optoelectronic properties and excellent robustness in photovoltaic devices. However, charge extraction/transport and ultimate power conversion efficiency (PCE) in 2D perovskite solar cells (PSCs) are still limited by the non‐eliminable quantum well effect. Here, a slow post‐annealing (SPA) process is proposed for BA2MA3Pb4I13 (n = 4) 2D PSCs by which a champion PCE of 17.26% is achieved with simultaneously enhanced open‐circuit voltage, short‐circuit current, and fill factor. Investigation with optical spectroscopy coupled with structural analyses indicates that enhanced crystal orientation and favorable alignment on the multiple perovskite phases (from the 2D phase near bottom to quasi‐3D phase near top regions) is obtained with SPA treatment, which promotes carrier transport/extraction and suppresses Shockley–Read–Hall charge recombination in the solar cell. As far as it is known, the reported PCE is so far the highest efficiency in RP phase 2D PSCs based on butylamine (BA) spacers (n = 4). The SPA‐processed devices exhibit a satisfactory stability with <4.5% degradation after 2000 h under N2 environment without encapsulation. The demonstrated process strategy offers a promising route to push forward the performance in 2D PSCs toward realistic photovoltaic applications.
The small-world organization has been hypothesized to reflect a balance between local processing and global integration in the human brain. Previous multimodal imaging studies have consistently demonstrated that the topological architecture of the brain network is disrupted in Alzheimer's disease (AD). However, these studies have reported inconsistent results regarding the topological properties of brain alterations in AD. One potential explanation for these inconsistent results lies with the diverse homogeneity and distinct progressive stages of the AD involved in these studies, which are thought to be critical factors that might affect the results. We investigated the topological properties of brain functional networks derived from resting functional magnetic resonance imaging (fMRI) of carefully selected moderate AD patients and normal controls (NCs). Our results showed that the topological properties were found to be disrupted in AD patients, which showing increased local efficiency but decreased global efficiency. We found that the altered brain regions are mainly located in the default mode network, the temporal lobe and certain subcortical regions that are closely associated with the neuropathological changes in AD. Of note, our exploratory study revealed that the ApoE genotype modulates brain network properties, especially in AD patients.
The Li-Mg-B-H system that is prepared from 2LiH + MgB 2 or 2LiBH 4 + MgH 2 possesses high hydrogen capacity and relatively favorable thermodynamics, but it is greatly restricted in practical hydrogen storage applications by problematic H-exchange kinetics. In the present study, TiF 3 was mechanically milled with a 2LiH + MgB 2 mixture and examined with respect to its effect on reversible dehydrogenation of the Li-Mg-B-H system. Experimental study showed that TiF 3 is highly effective for promoting the two-step dehydrogenation reaction in the Li-Mg-B-H system. Compared to the neat 2LiH + MgB 2 sample, the 2LiH + MgB 2 + 0.01TiF 3 sample exhibits significantly reduced dehydrogenation temperature and markedly enhanced dehydriding rate at both steps. Furthermore, the catalytic enhancement arising upon adding TiF 3 additive was observed to persist well in the hydrogenation/dehydrogenation cycles. Based on the results of phase analysis and a series of designed experiments, the mechanism underlying the observed property improvement is discussed.
Identification of early-stage pulmonary adenocarcinomas before surgery, especially in cases of subcentimeter cancers, would be clinically important and could provide guidance to clinical decision making. In this study, we developed a deep learning system based on 3D convolutional neural networks and multitask learning, which automatically predicts tumor invasiveness, together with 3D nodule segmentation masks. The system processes a 3D nodule-centered patch of preprocessed CT and learns a deep representation of a given nodule without the need for any additional information. A dataset of 651 nodules with manually segmented voxel-wise masks and pathological labels of atypical adenomatous hyperplasia (AAH), adenocarcinomas in situ (AIS), minimally invasive adenocarcinoma (MIA), and invasive pulmonary adenocarcinoma (IA) was used in this study. We trained and validated our deep learning system on 523 nodules and tested its performance on 128 nodules. An observer study with 2 groups of radio-logists, 2 senior and 2 junior, was also investigated. We merged AAH and AIS into one single category AAH-AIS, comprising a 3-category classification in our study. The proposed deep learning system achieved better classification performance than the radiologists; in terms of 3-class weighted average F1 score, the model achieved 63.3% while the radiologists achieved 55.6%, 56.6%, 54.3%, and 51.0%, respectively. These results suggest that deep learning methods improve the yield of discriminative results and hold promise in the CADx application domain, which could help doctors work efficiently and facilitate the application of precision medicine.Significance: Machine learning tools are beginning to be implemented for clinical applications. This study represents an important milestone for this emerging technology, which could improve therapy selection for patients with lung cancer.
Solution‐processed metal‐based halide perovskites have taken a dominant position for perovskite optoelectronics including light emission and X‐ray detection; however, the toxicity of the included heavy metals severely restricts their applications for wearable, lightweight, and transient optoelectronic devices. Here, the authors describe investigations of large (4 × 6 × 2 mm3) 3D metal‐free perovskite MDABCO‐NH4I3 (MDBACO = methyl‐N′‐diazabicyclo[2.2.2]octonium) single crystal and its charge recombination and extraction behavior for light emission and X‐ray detection. Unlike conventional 3D metal‐based perovskites, this lightweight and biocompatible perovskite large crystal is processed from aqueous solution at room temperature, and can achieve both an extremely long carrier lifetime up to ≈1.03 µs and the formation of self‐trapped excited states for luminescence. These features contribute to a photoluminescence quantum yield (PLQY) as high as ≈53% at room temperature and an X‐ray sensitivity up to 1997 ± 80 μC Gy cm−2 at 50 V bias (highest among all metal‐free detectors). The ability to tune the perovskite band gap by modulating the structure under high pressure is also demonstrated, which opens up applications for the crystal as colored emitters. These attributes make it a molecular alternative to metal‐based perovskites for biocompatible and transient optoelectronics.
Even though the perovskite solar cell has been so popular for its skyrocketing power conversion efficiency, its further development is still roadblocked by its overall performance, in particular long-term stability, large-area fabrication and stable module efficiency. In essence, the soft component and ionic–electronic nature of metal halide perovskites usually chaperonage large number of anion vacancy defects that act as recombination centers to decrease both the photovoltaic efficiency and operational stability. Herein, we report a one-stone-for-two-birds strategy in which both anion-fixation and associated undercoordinated-Pb passivation are in situ achieved during crystallization by using a single amidino-based ligand, namely 3-amidinopyridine, for metal-halide perovskite to overcome above challenges. The resultant devices attain a power conversion efficiency as high as 25.3% (certified at 24.8%) with substantially improved stability. Moreover, the device without encapsulation retained 92% of its initial efficiency after 5000 h exposure in ambient and the device with encapsulation retained 95% of its initial efficiency after >500 h working at the maximum power point under continuous light irradiation in ambient. It is expected this one-stone-for-two-birds strategy will benefit large-area fabrication that desires for simplicity.
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