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Asymmetric Nanoparticle Oxidation Observed In-Situ by the Evolution of Diffraction Contrast 用衍射对比的演化方法原位观察不对称纳米颗粒氧化
3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-10-01 DOI: 10.1088/2515-7639/ad025f
Agus Riyanto Poerwoprajitno, Nitish Baradwaj, Manish Kumar Singh, C. Barry Carter, Dale Huber, Rajiv Kalia, John Watt
Abstract The use of transmission electron microscopy (TEM) to observe real-time structural and compositional changes has proven to be a valuable tool for understanding the dynamic behavior of nanomaterials. However, identifying the nanoparticles of interest typically require an obvious change in position, size, or structure, as compositional changes may not be noticeable during the experiment. Oxidation or reduction can often result in subtle volume changes only, so elucidating mechanisms in real-time requires atomic-scale resolution or in-situ electron energy loss spectroscopy, which may not be widely accessible. Here, by monitoring the evolution of diffraction contrast, we can observe both structural and compositional changes in iron oxide nanoparticles, specifically the oxidation from a wüstite-magnetite (FeO@Fe 3 O 4 ) core – shell nanoparticle to single crystalline magnetite, Fe 3 O 4 nanoparticle. The in-situ TEM images reveal a distinctive light and dark contrast known as the ‘Ashby-Brown contrast’, which is a result of coherent strain across the core – shell interface. As the nanoparticles fully oxidize to Fe 3 O 4 , the diffraction contrast evolves and then disappears completely, which is then confirmed by modeling and simulation of TEM images. This represents a new, simplified approach to tracking the oxidation or reduction mechanisms of nanoparticles using in-situ TEM experiments.
摘要:利用透射电子显微镜(TEM)实时观察纳米材料的结构和组成变化已被证明是了解纳米材料动态行为的一种有价值的工具。然而,识别感兴趣的纳米颗粒通常需要在位置、大小或结构上有明显的变化,因为在实验过程中成分的变化可能不明显。氧化或还原通常只会导致微小的体积变化,因此实时阐明机制需要原子尺度的分辨率或原位电子能量损失光谱,这可能不是很容易获得。通过监测衍射对比的演变,我们可以观察到氧化铁纳米颗粒的结构和成分的变化,特别是从w石-磁铁矿(FeO@Fe 3o4)核-壳纳米颗粒氧化到单晶磁铁矿,fe3o4纳米颗粒。原位TEM图像显示了一种独特的明暗对比,称为“Ashby-Brown对比”,这是核-壳界面上相干应变的结果。当纳米颗粒完全氧化为fe3o4时,衍射对比发生变化,然后完全消失,并通过TEM图像的建模和模拟证实了这一点。这代表了一种新的、简化的方法来跟踪纳米颗粒的氧化或还原机制,使用原位透射电镜实验。
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引用次数: 0
In situ XPS of Competitive CO2/H2O Absorption in an Ionic Liquid 离子液体中竞争性CO2/H2O吸收的原位XPS
3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-10-01 DOI: 10.1088/2515-7639/acfdcf
Jordan Cole, Zoe Henderson, Andrew G Thomas, Christopher Castle, Adam Greer, Christopher Hardacre, Mattia Scardamaglia, Andrey Shavorskiy, Karen Louise Syres
Abstract Superbasic ionic liquids (SBILs) are being investigated as potential carbon dioxide (CO 2 ) gas capture agents, however, the presence of H 2 O in the flue stream can inhibit the uptake of CO 2 . In this study a thin film of the SBIL trihexyltetradecylphosphonium 1,2,4-triazolide ([P 66614 ][124Triz]) was deposited onto rutile TiO 2 (110) using in situ electrospray deposition and studied upon exposure to CO 2 and H 2 O using in situ near-ambient pressure x-ray photoelectron spectroscopy (NAP-XPS). The molar uptake ratio of gas in the electrosprayed SBIL ( n gas :n IL ) was calculated to be 0.3:1 for CO 2 , 0.7:1 for H 2 O, and 0.9:1 for a CO 2 /H 2 O mixture. NAP-XPS taken at two different depths reveals that the competitive absorption of CO 2 and H 2 O in [P 66614 ][124Triz] varies with sampling depth. A greater concentration of CO 2 absorbs in the bulk layers, while more H 2 O adsorbs/absorbs at the surface. The presence of H 2 O in the gas mixture does not inhibit the absorption of CO 2 . Measurements taken during exposure and after the removal of gas indicate that CO 2 absorbed in the bulk does so reversibly, whilst CO 2 adsorbed/absorbed at the surface does so irreversibly. This is contrary to the fully reversible CO 2 reaction shown for bulk ionic liquids (ILs) in literature and suggests that irreversible absorption of CO 2 in our highly-structured thin films is largely attributed to reactions at the surface. This has potential implications on IL gas capture and thin film IL catalysis applications.
超碱性离子液体(SBILs)作为潜在的二氧化碳气体捕集剂正在被研究,然而,烟道流中h2o的存在会抑制CO 2的吸收。在本研究中,采用原位电喷雾沉积方法将三己基四烷基膦1,2,4-三唑烷([P 66614][124Triz])薄膜沉积在金红石tio2(110)上,并使用近环境压力x射线光电子能谱(napp - xps)研究了暴露于CO 2和h2o的情况。经计算得出,在电喷涂的SBIL (n气体:n IL)中,co2的摩尔吸收比为0.3:1,h2o的摩尔吸收比为0.7:1,co2 / h2o混合物的摩尔吸收比为0.9:1。两种不同深度的NAP-XPS表明,[p66614][124Triz]中CO 2和h2o的竞争吸收随采样深度的变化而变化。较大浓度的co2在主体层中被吸收,而较多的h2o在表层被吸收。混合气体中h2o的存在并不会抑制co2的吸收。在暴露期间和去除气体后进行的测量表明,co2在主体中被吸收是可逆的,而co2在表面被吸附/吸收是不可逆的。这与文献中大块离子液体(ILs)的完全可逆CO 2反应相反,表明我们的高结构薄膜中CO 2的不可逆吸收主要归因于表面的反应。这对IL气体捕获和薄膜IL催化应用具有潜在的意义。
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引用次数: 0
Intrinsic thermal expansion and tunability of thermal expansion coefficient in Ni-substituted Co2V2O7 ni取代Co2V2O7的固有热膨胀和热膨胀系数的可调性
3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-10-01 DOI: 10.1088/2515-7639/acfdce
Erica T Esteban, Jasmine J Garcia, Sophie R Windover, Joya Cooley
Abstract Framework oxide materials are well-known for exhibiting not only negative thermal expansion (NTE), but also demonstrating thermal expansion that can be controlled using composition as a tuning parameter. In this work, we study the intrinsic thermal expansion properties of Co 2 V 2 O 7 , which has shown bulk linear NTE, and attempt to understand how substituting Ni 2+ for Co 2+ will affect the thermal expansion. The isomorphic solid solution is synthesized through solid-state methods and characterized using x-ray diffraction (XRD), diffuse reflectance spectroscopy, and neutron diffraction. The size difference between Ni 2+ and Co 2+ as well as the polyhedral volume of each Co 2+ metal coordination environment in the crystal structure allows Ni 2+ to partially be directed toward one crystallographic site over the other. Variable temperature synchrotron XRD data are employed to understand intrinsic thermal expansion. Across the solid solution, no intrinsic NTE is observed at the microscopic level, yet a degree of tunability in the thermal expansion coefficient with Ni substitution is demonstrated. The disparities between the intrinsic and bulk thermal expansion properties suggest that a morphological mechanism may have resulted in NTE in the bulk.
摘要框架氧化物材料不仅表现出负热膨胀(NTE),而且表现出可以使用成分作为调谐参数来控制的热膨胀。在这项工作中,我们研究了co2v2o7的固有热膨胀性质,它已经显示出大块线性NTE,并试图了解用Ni 2+代替Co 2+将如何影响热膨胀。采用固相法合成了该同构固溶体,并用x射线衍射(XRD)、漫反射光谱和中子衍射对其进行了表征。Ni 2+和Co 2+之间的尺寸差异以及晶体结构中每种Co 2+金属配位环境的多面体体积允许Ni 2+部分地指向一个晶体位置而不是另一个晶体位置。采用变温同步加速器XRD数据来理解本征热膨胀。在整个固溶体中,在微观水平上没有观察到本征的NTE,但在Ni取代的热膨胀系数中有一定程度的可调性。本征热膨胀性能和体体热膨胀性能之间的差异表明,形态机制可能导致了体的NTE。
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引用次数: 0
Recent Developments in Non-Fullerene-Acceptor-Based Indoor Organic Solar Cells 基于非富勒烯受体的室内有机太阳能电池的最新进展
3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-10-01 DOI: 10.1088/2515-7639/ad01df
Swarup Biswas, Yongju Lee, Hyojeong Choi, Hyeok Kim
Abstract For over a decade, donor-acceptor blends composed of organic donors and fullerene acceptors dominated indoor organic solar cells (IOSCs). Numerous researchers have invested time to conduct extensive studies on developing new donor acceptor materials, interlayers, minimizing energy losses, and enhancing the open-circuit voltage ( V OC ) through device and material engineering, and optimizing device architectures to achieve highly efficient, environmentally stable, and commercially acceptable IOSCs. Through such efforts, the maximum power conversion efficiencies (PCEs) of IOSCs have surpassed 35%. In this regard, the transition from a fullerene to non-fullerene acceptor (NFA) is a useful strategy for enhancing the PCEs of IOSCs by allowing adjustment of the energy levels for compatibility with the indoor light spectrum and by improving photon absorption in the visible range, thereby boosting photocurrent generation and enhancing V OC . NFA-based indoor organic photovoltaic systems have recently drawn interest from the scholarly community. To compete with the standard batteries used in the Internet of Things devices, additional research is needed to enhance several characteristics, including manufacturing costs and device longevity, which must maintain at least 80% of their initial PCEs for more than 10 years. Further development in this field can greatly benefit from a thorough and comprehensive review on this field. Hence, this review explores recent advances in IOSCs systems based on NFAs. First, we explain several methods used to create extremely effective IOSCs, IOSCs based on fullerene acceptors are next reviewed and discussed. The disadvantages of using fullerene acceptors in IOSCs are noted. Then, we introduce NFAs and explore existing research on the subject. Finally, we discuss the commercial potential of NFA-based IOSCs and their future outlook.
十多年来,由有机供体和富勒烯受体组成的供体-受体混合物主导了室内有机太阳能电池(IOSCs)。许多研究人员投入了大量时间进行广泛的研究,开发新的供体受体材料,中间层,通过器件和材料工程最小化能量损失,提高开路电压(V OC),并优化器件架构,以实现高效,环境稳定和商业上可接受的IOSCs。通过这些努力,IOSCs的最大功率转换效率(pce)已超过35%。在这方面,从富勒烯到非富勒烯受体(NFA)的转变是提高IOSCs pce的有用策略,通过允许调整与室内光谱的兼容性的能级,并通过改善可见光范围内的光子吸收,从而促进光电流的产生和提高V OC。基于nfa的室内有机光伏系统最近引起了学术界的兴趣。为了与物联网设备中使用的标准电池竞争,需要进一步的研究来提高几个特性,包括制造成本和设备寿命,设备必须保持至少80%的初始pce超过10年。对这一领域进行彻底和全面的审查将大大有利于这一领域的进一步发展。因此,本文综述了基于NFAs的IOSCs系统的最新进展。首先,我们解释了几种用于创建非常有效的IOSCs的方法,接下来将对基于富勒烯受体的IOSCs进行回顾和讨论。指出了在IOSCs中使用富勒烯受体的缺点。然后,我们介绍了NFAs,并对该主题的现有研究进行了探讨。最后,我们讨论了基于nfa的IOSCs的商业潜力及其未来前景。
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引用次数: 0
Machine learning (ML)-assisted surface tension and oscillation-induced elastic modulus studies of oxide-coated liquid metal (LM) alloys. 机器学习(ML)辅助氧化物涂层液态金属(LM)合金的表面张力和振荡诱导弹性模量研究。
IF 4.8 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-10-01 Epub Date: 2023-09-26 DOI: 10.1088/2515-7639/acf78c
Kazi Zihan Hossain, Sharif Amit Kamran, Alireza Tavakkoli, M Rashed Khan

Pendant drops of oxide-coated high-surface tension fluids frequently produce perturbed shapes that impede interfacial studies. Eutectic gallium indium or Galinstan are high-surface tension fluids coated with a ∼5 nm gallium oxide (Ga2O3) film and falls under this fluid classification, also known as liquid metals (LMs). The recent emergence of LM-based applications often cannot proceed without analyzing interfacial energetics in different environments. While numerous techniques are available in the literature for interfacial studies- pendant droplet-based analyses are the simplest. However, the perturbed shape of the pendant drops due to the presence of surface oxide has been ignored frequently as a source of error. Also, exploratory investigations of surface oxide leveraging oscillatory pendant droplets have remained untapped. We address both challenges and present two contributing novelties- (a) by utilizing the machine learning (ML) technique, we predict the approximate surface tension value of perturbed pendant droplets, (ii) by leveraging the oscillation-induced bubble tensiometry method, we study the dynamic elastic modulus of the oxide-coated LM droplets. We have created our dataset from LM's pendant drop shape parameters and trained different models for comparison. We have achieved >99% accuracy with all models and added versatility to work with other fluids. The best-performing model was leveraged further to predict the approximate values of the nonaxisymmetric LM droplets. Then, we analyzed LM's elastic and viscous moduli in air, harnessing oscillation-induced pendant droplets, which provides complementary opportunities for interfacial studies alternative to expensive rheometers. We believe it will enable more fundamental studies of the oxide layer on LM, leveraging both symmetric and perturbed droplets. Our study broadens the materials science horizon, where researchers from ML and artificial intelligence domains can work synergistically to solve more complex problems related to surface science, interfacial studies, and other studies relevant to LM-based systems.

氧化物涂层的高表面张力流体的悬滴经常产生扰动形状,阻碍界面研究。共晶镓铟或Galinstan是涂有~5 nm氧化镓(Ga2O3)膜的高表面张力流体,属于这种流体分类,也称为液态金属(LMs)。最近出现的基于LM的应用通常不能在不分析不同环境中的界面能量学的情况下进行。虽然文献中有许多技术可用于界面研究,但基于悬滴的分析是最简单的。然而,由于表面氧化物的存在,悬滴的扰动形状经常被忽视,成为误差的来源。此外,利用振荡悬滴的表面氧化物的探索性研究尚未开发。我们解决了这两个挑战,并提出了两个有贡献的新颖性——(a)通过利用机器学习(ML)技术,我们预测了扰动垂向液滴的近似表面张力值;(ii)通过利用振荡诱导气泡张力计方法,我们研究了氧化物涂层LM液滴的动态弹性模量。我们根据LM的垂坠形状参数创建了数据集,并训练了不同的模型进行比较。我们在所有型号中都实现了>99%的准确率,并增加了与其他流体配合使用的多功能性。进一步利用性能最佳的模型来预测非轴对称LM液滴的近似值。然后,我们分析了LM在空气中的弹性和粘性模量,利用振荡诱导的垂向液滴,这为界面研究提供了替代昂贵流变仪的补充机会。我们相信,它将利用对称液滴和扰动液滴,对LM上的氧化物层进行更基础的研究。我们的研究拓宽了材料科学的视野,来自ML和人工智能领域的研究人员可以协同工作,解决与表面科学、界面研究和其他与基于LM的系统相关的研究相关的更复杂的问题。
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引用次数: 0
Universal material trends in extraordinary magnetoresistive devices 特殊磁阻器件的通用材料趋势
3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-09-29 DOI: 10.1088/2515-7639/acfac0
Ricci Erlandsen, Thierry Désiré Pomar, Lior Kornblum, Nini Pryds, Rasmus Bjørk, Dennis Valbjørn Christensen
Abstract Extraordinary magnetoresistance (EMR) is a geometric magnetoresistance emerging in hybrid systems typically comprising a high-mobility material and a metal. Due to a field-dependent redistribution of electrical currents in these devices, the electrical resistance at room temperature can increase by 10 7 % when applying a magnetic field of 5 T. Although EMR holds considerable potential for realizing sensitive, all-electronic magnetometers, this potential is largely unmet. A key challenge is that the performance of EMR devices depends very sensitively on variations in a vast parameter space where changes in the device geometry and material properties produce widely different EMR performances. The challenge of navigating in the large parameter space is further amplified by the poor understanding of the interplay between the device geometry and material properties. By systematically varying the material parameters in four key EMR geometries using diffusive transport simulations, we here elucidate this interplay with the aim of finding universal guidelines for designing EMR devices. Common to all geometries, we find that the sensitivity scales inversely with the carrier density, while the MR reaches saturation at low carrier densities. Increasing the mobility beyond 20 000 cm 2 Vs −1 is required to observe strong EMR effects at 1 T with the optimal magnetoresistance observed for mobilities between 100 000–500 000 cm 2 Vs −1 . An interface resistance below ρ c = 10 4 Ω cm 2 between the constituent materials in the hybrid devices was also found to be a prerequisite for very high magnetoresistances in all geometries. By further simulating several high-mobility materials at room and cryogenic temperatures, we conclude that encapsulated graphene and InSb are amongst the most promising candidates for EMR devices showing high magnetoresistance exceeding 10 7 % below 1 T at room temperature. This study paves the way for understanding how to realize EMR devices with record-high magnetoresistance and high sensitivity for detecting magnetic fields.
异常磁阻(EMR)是一种出现在混合系统中的几何磁阻,通常由高迁移率材料和金属组成。由于这些器件中电流的场依赖性再分布,当施加5 t的磁场时,室温下的电阻可以增加10.7%。尽管EMR具有实现灵敏的全电子磁强计的巨大潜力,但这一潜力在很大程度上没有得到满足。一个关键的挑战是,EMR器件的性能非常敏感地取决于巨大参数空间的变化,其中器件几何形状和材料特性的变化会产生截然不同的EMR性能。由于对器件几何形状和材料特性之间相互作用的理解不足,在大参数空间中导航的挑战进一步扩大。通过使用扩散输运模拟系统地改变四种关键EMR几何形状中的材料参数,我们在这里阐明了这种相互作用,目的是找到设计EMR器件的通用指南。与所有几何形状一样,我们发现灵敏度与载流子密度成反比,而MR在低载流子密度下达到饱和。要在1 T下观察到强EMR效应,需要将迁移率提高到20,000 cm 2 v−1以上,而在100,000 - 500,000 cm 2 v−1之间的迁移率观察到最佳磁电阻。混合器件中组成材料之间的界面电阻低于ρ c = 10−4 Ω cm 2,这也是在所有几何形状中获得非常高磁阻的先决条件。通过进一步在室温和低温下模拟几种高迁移率材料,我们得出结论,封装石墨烯和InSb是EMR器件最有希望的候选者之一,在室温下,在1 T以下显示出超过10.7%的高磁阻。该研究为了解如何实现具有创纪录高磁阻和高灵敏度的EMR器件奠定了基础。
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引用次数: 0
Biomaterials Interventions for Pelvic Organ Prolapse. 盆腔器官脱垂的生物材料干预。
IF 4.8 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2023-01-01
Katrina M Knight
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引用次数: 0
Turn of the decade: versatility of 2D hexagonal boron nitride. 世纪之交:二维六方氮化硼的多功能性。
IF 4.9 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2021-01-01 DOI: 10.1088/2515-7639/abf1ab
Albert F Rigosi, Antonio L Levy, Michael R Snure, Nicholas R Glavin

The era of two-dimensional (2D) materials, in its current form, truly began at the time that graphene was first isolated just over 15 years ago. Shortly thereafter, the use of 2D hexagonal boron nitride (h-BN) had expanded in popularity, with use of the thin isolator permeating a significant number of fields in condensed matter and beyond. Due to the impractical nature of cataloguing every use or research pursuit, this review will cover ground in the following three subtopics relevant to this versatile material: growth, electrical measurements, and applications in optics and photonics. Through understanding how the material has been utilized, one may anticipate some of the exciting directions made possible by the research conducted up through the turn of this decade.

目前形式的二维(2D)材料时代真正开始于15年前石墨烯首次被分离的时候。此后不久,2D六方氮化硼(h-BN)的使用越来越受欢迎,薄隔离器的使用渗透到凝聚态及其他领域的大量领域。由于对每一种用途或研究追求进行编目的不切实际性,本综述将涵盖与这种多用途材料相关的以下三个子主题:生长、电学测量以及光学和光子学应用。通过了解这种材料是如何被利用的,人们可以预测到本十年之交进行的研究所带来的一些令人兴奋的方向。
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引用次数: 0
Large area few-layer TMD film growths and their applications. 大面积少层TMD薄膜生长及其应用。
IF 4.8 3区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2020-04-01 Epub Date: 2020-04-27 DOI: 10.1088/2515-7639/ab82b3
Srinivas V Mandyam, Hyong M Kim, Marija Drndić

Research on 2D materials is one of the core themes of modern condensed matter physics. Prompted by the experimental isolation of graphene, much attention has been given to the unique optical, electronic, and structural properties of these materials. In the past few years, semiconducting transition metal dichalcogenides (TMDs) have attracted increasing interest due to properties such as direct band gaps and intrinsically broken inversion symmetry. Practical utilization of these properties demands large-area synthesis. While films of graphene have been by now synthesized on the order of square meters, analogous achievements are difficult for TMDs given the complexity of their growth kinetics. This article provides an overview of methods used to synthesize films of mono- and few-layer TMDs, comparing spatial and time scales for the different growth strategies. A special emphasis is placed on the unique applications enabled by such large-scale realization, in fields such as electronics and optics.

二维材料的研究是现代凝聚态物理的核心主题之一。由于石墨烯的实验分离,这些材料独特的光学、电子和结构特性引起了人们的广泛关注。在过去的几年中,半导体过渡金属二硫族化合物(TMDs)由于其直接带隙和本质破缺反转对称性等特性而引起了人们越来越多的兴趣。这些性质的实际应用需要大面积合成。虽然目前石墨烯薄膜的合成已经达到了平方米量级,但由于其生长动力学的复杂性,tmd很难取得类似的成就。本文综述了单层和多层tmd薄膜的合成方法,并对不同生长策略的空间和时间尺度进行了比较。特别强调的是这种大规模实现在电子和光学等领域的独特应用。
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引用次数: 26
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