All‐inorganic CsPbI3quantum dots (QDs) have shown great potential in photovoltaic applications. However, their performance has been limited by defects and phase stability. Herein, an anion/cation synergy strategy to improve the structural stability of CsPbI3QDs and reduce the pivotal iodine vacancy (
Volumetric defect types commonly observed in the additively manufactured parts differ in their morphologies ascribed to their formation mechanisms. Using high-resolution X-ray computed tomography, this study analyzes the morphological features of volumetric defects, and their statistical distribution, in laser powder bed fused Ti-6Al-4V. The geometries of three common types of volumetric defects; i.e., lack of fusions, gas-entrapped pores, and keyholes, are quantified by nine parameters including maximum dimension, roundness, sparseness, aspect ratio, and more. It is shown that the three defect types share overlaps of different degrees in the ranges of their morphological parameters; thus, employing only one or two parameters cannot uniquely determine a defect’s type. To overcome this challenge, a defect classification methodology incorporating multiple morphological parameters has been proposed. In this work, by employing the most discriminating parameters, this methodology has been shown effective when implemented into decision tree (>98% accuracy) and artificial neural network (>99% accuracy).
more » « less- NSF-PAR ID:
- 10377079
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 13
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract V I) defect states is proposed. The Zn‐doped CsPbI3(Zn:CsPbI3) QDs have been successfully synthesized employing ZnI2as the dopant to provide Zn2+and extra I−. Theoretical calculations and experimental results demonstrate that the Zn:CsPbI3QDs show better thermodynamic stability and higher photoluminescence quantum yield (PLQY) compared to the pristine CsPbI3QDs. The doping of Zn in CsPbI3QDs increases the formation energy and Goldschmidt tolerance factor, thereby improving the thermodynamic stability. The additional I−helps to reduce theV Idefects during the synthesis of CsPbI3QDs, resulting in the higher PLQY. More importantly, the synergistic effect of Zn2+and I−in CsPbI3QDs can prevent the iodine loss during the fabrication of CsPbI3QD film, inhibiting the formation of newV Idefect states in the construction of solar cells. Consequently, the anion/cation synergy strategy affords the CsPbI3quantum dot solar cells (QDSC) a power conversion efficiency over 16%, which is among the best efficiencies for perovskite QDSCs. -
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Abstract Purpose The interaction between129Xe atoms and pulmonary capillary red blood cells provides cardiogenic signal oscillations that display sensitivity to precapillary and postcapillary pulmonary hypertension. Recently, such oscillations have been spatially mapped, but little is known about optimal reconstruction or sensitivity to artifacts. In this study, we use digital phantom simulations to specifically optimize keyhole reconstruction for oscillation imaging. We then use this optimized method to re‐establish healthy reference values and quantitatively evaluate microvascular flow changes in patients with chronic thromboembolic pulmonary hypertension (CTEPH) before and after pulmonary thromboendarterectomy (PTE).
Methods A six‐zone digital lung phantom was designed to investigate the effects of radial views, key radius, and SNR. One‐point Dixon129Xe gas exchange MRI images were acquired in a healthy cohort (
n = 17) to generate a reference distribution and thresholds for mapping red blood cell oscillations. These thresholds were applied to 10 CTEPH participants, with 6 rescanned following PTE.Results For undersampled acquisitions, a key radius of was found to optimally resolve oscillation defects while minimizing excessive heterogeneity. CTEPH participants at baseline showed higher oscillation defect + low (32 ± 14%) compared with healthy volunteers (18 ± 12%,
p < 0.001). For those scanned both before and after PTE, oscillation defect + low decreased from 37 ± 13% to 23 ± 14% (p = 0.03).Conclusions Digital phantom simulations have informed an optimized keyhole reconstruction technique for gas exchange images acquired with standard 1‐point Dixon parameters. Our proposed methodology enables more robust quantitative mapping of cardiogenic oscillations, potentially facilitating effective regional quantification of microvascular flow impairment in patients with pulmonary vascular diseases such as CTEPH.
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Three typical types of defects, i.e., keyholes, lack of fusion (LoF), and gas-entrapped pores (GEP), characterized by various features (e.g., volume, surface area, etc.), are generated under different process parameters of laser beam powder bed fusion (L-PBF) processes in additive manufacturing (AM). The different types of defects deteriorate the mechanical performance of L- PBF components, such as fatigue life, to a different extent. However, there is a lack of recognized approaches to classify the defects automatically and accurately in L-PBF components. This work presents a novel hierarchical graph convolutional network (H-GCN) to classify different types of defects by a cascading GCN structure with a low-level feature (e.g., defect features) layer and a high-level feature (e.g., process parameters) layer. Such an H-GCN not only leverages the multi- level information from process parameters and defect features to classify the defects but also explores the impact of process parameters on defect types and features. The H-GCN is evaluated through a case study with X-ray computed tomography (CT) L-PBF defect datasets and compared with several machine learning methods. H-GCN exhibits an outstanding classification performance with an F1-score of 1.000 and reveals the potential effect of process parameters on three types of defects.more » « less
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Neurotransmitters are small molecules involved in neuronal signaling and can also serve as stress biomarkers.1Their abnormal levels have been also proposed to be indicative of several neurological diseases such as Alzheimer’s disease, Parkinson’s disease, Huntington disease, among others. Hence, measuring their levels is highly important for early diagnosis, therapy, and disease prognosis. In this work, we investigate facile functionalization methods to tune and enhance sensitivity of printed graphene sensors to neurotransmitters. Sensors based on direct laser scribing and screen-printed graphene ink are studied. These printing methods offer ease of prototyping and scalable fabrication at low cost.
The effect of functionalization of laser induced graphene (LIG) by electrodeposition and solution-based deposition of TMDs (molybdenum disulfide2and tungsten disulfide) and metal nanoparticles is studied. For different processing methods, electrochemical characteristics (such as electrochemically active surface area: ECSA and heterogenous electron transfer rate: k0) are extracted and correlated to surface chemistry and defect density obtained respectively using X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy. These functionalization methods are observed to directly impact the sensitivity and limit of detection (LOD) of the graphene sensors for the studied neurotransmitters. For example, as compared to bare LIG, it is observed that electrodeposition of MoS2on LIG improves ECSA by 3 times and k0by 1.5 times.3Electrodeposition of MoS2also significantly reduces LOD of serotonin and dopamine in saliva, enabling detection of their physiologically relevant concentrations (in pM-nM range). In addition, chemical treatment of LIG sensors is carried out in the form of acetic acid treatment. Acetic acid treatment has been shown previously to improve C-C bonds improving the conductivity of LIG sensors.4In our work, in particular, acetic acid treatment leads to larger improvement of LOD of norepinephrine compared to MoS2electrodeposition.
In addition, we investigate the effect of plasma treatment to tune the sensor response by modifying the defect density and chemistry. For example, we find that oxygen plasma treatment of screen-printed graphene ink greatly improves LOD of norepinephrine up to three orders of magnitude, which may be attributed to the increased defects and oxygen functional groups on the surface as evident by XPS measurements. Defects are known to play a key role in enhancing the sensitivity of 2D materials to surface interactions, and have been explored in tuning/enhancing the sensor sensitivity.5Building on our previous work,3we apply a custom machine learning-based data processing method to further improve that sensitivity and LOD, and also to automatically benchmark different molecule-material pairs.
Future work includes expanding the plasma chemistry and conditions, studying the effect of precursor mixture in laser-induced solution-based functionalization, and understanding the interplay between molecule-material system. Work is also underway to improve the machine learning model by using nonlinear learning models such as neural networks to improve the sensor sensitivity, selectivity, and robustness.
References A. J. Steckl, P. Ray, (2018), doi:10.1021/acssensors.8b00726.
Y. Lei, D. Butler, M. C. Lucking, F. Zhang, T. Xia, K. Fujisawa, T. Granzier-Nakajima, R. Cruz-Silva, M. Endo, H. Terrones, M. Terrones, A. Ebrahimi,
Sci. Adv. 6 , 4250–4257 (2020).V. Kammarchedu, D. Butler, A. Ebrahimi,
Anal. Chim. Acta .1232 , 340447 (2022).H. Yoon, J. Nah, H. Kim, S. Ko, M. Sharifuzzaman, S. C. Barman, X. Xuan, J. Kim, J. Y. Park,
Sensors Actuators B Chem. 311 , 127866 (2020).T. Wu, A. Alharbi, R. Kiani, D. Shahrjerdi,
Adv. Mater. 31 , 1–12 (2019). -
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Thin solids often develop elastic instabilities and subsequently complex, multiscale deformation patterns. Revealing the organizing principles of this spatial complexity has ramifications for our understanding of morphogenetic processes in plant leaves and animal epithelia and perhaps even the formation of human fingerprints. We elucidate a primary source of this morphological complexity—an incompatibility between an elastically favored “microstructure” of uniformly spaced wrinkles and a “macrostructure” imparted through the wrinkle director and dictated by confinement forces. Our theory is borne out of experiments and simulations of floating sheets subjected to radial stretching. By analyzing patterns of grossly radial wrinkles we find two sharply distinct morphologies: defect-free patterns with a fixed number of wrinkles and nonuniform spacing and patterns of uniformly spaced wrinkles separated by defect-rich buffer zones. We show how these morphological types reflect distinct minima of a Ginzburg–Landau functional—a coarse-grained version of the elastic energy, which penalizes nonuniform wrinkle spacing and amplitude, as well as deviations of the actual director from the axis imposed by confinement. Our results extend the effective description of wrinkle patterns as liquid crystals [H. Aharoni
et al .,Nat. Commun. 8, 15809 (2017)], and we highlight a fascinating analogy between the geometry–energy interplay that underlies the proliferation of defects in the mechanical equilibrium of confined sheets and in thermodynamic phases of superconductors and chiral liquid crystals.
