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Universal Synthesis of Core–Shell-Structured Ordered Mesoporous Transition Metal Dichalcogenides/Metal Oxides Heterostructures with Active Edge Sites 具有活性边缘位点的核壳结构有序介孔过渡金属二卤化物/金属氧化物异质结构的通用合成方法
Pub Date : 2024-09-04 DOI: 10.1002/sstr.202400376
Zhenliang Li, Yujian Rao, Zhehan Wang, Tuo Zhang, Guodong Wu, Litao Sun, Yuan Ren, Li Tao
Two-dimensional (2D) transition metal dichalcogenides (TMDs) are widely used in interfacial reactions and electronic devices due to their tunable bandgap and high efficiency of carrier transport. However, the lack of fully exposed active sites in bulk samples or stacked nanosheets leads to limited performances. In this work, a general method is developed to construct ordered mesoporous TMDs/metal oxides (OM-TMDs/MOs) heterostructures, including WS<sub>2</sub>/WO<sub>3</sub>, WSe<sub>2</sub>/WO<sub>3</sub>, WTe<sub>2</sub>/WO<sub>3</sub>, MoS<sub>2</sub>/MoO<sub>3</sub>, and V<sub>3</sub>S<sub>4</sub>/V<sub>2</sub>O<sub>3</sub>, through one-step thermal sulfurization (selenidation/tellurization) of self-assembled amphiphilic block copolymer/polyoxometalates clusters nanocomposites with ordered mesostructures. The OM-TMDs/MOs possess highly OM structures with high specific surface area, large pore size, and rich active edge sites in the frameworks of heterostructures. The chemiresistive gas sensor based on OM-WS<sub>2</sub>/WO<sub>3</sub> shows excellent NO<sub>2</sub>-sensing performances at room temperature, with high sensitivity, ultrahigh selectivity (<span data-altimg="/cms/asset/a3e5cd6e-ac04-41a3-b6e2-cce80c9d4d74/sstr202400376-math-0001.png"></span><mjx-container ctxtmenu_counter="3" ctxtmenu_oldtabindex="1" jax="CHTML" role="application" sre-explorer- style="font-size: 103%; position: relative;" tabindex="0"><mjx-math aria-hidden="true" location="graphic/sstr202400376-math-0001.png"><mjx-semantics><mjx-mrow><mjx-msub data-semantic-children="0,3" data-semantic- data-semantic-role="latinletter" data-semantic-speech="upper S Subscript NO Sub Subscript 2" data-semantic-type="subscript"><mjx-mi data-semantic-annotation="clearspeak:simple" data-semantic-font="italic" data-semantic- data-semantic-parent="4" data-semantic-role="latinletter" data-semantic-type="identifier"><mjx-c></mjx-c></mjx-mi><mjx-script style="vertical-align: -0.15em; margin-left: -0.032em;"><mjx-mrow size="s"><mjx-msub data-semantic-children="1,2" data-semantic- data-semantic-parent="4" data-semantic-role="unknown" data-semantic-type="subscript"><mjx-mrow><mjx-mtext data-semantic-annotation="clearspeak:unit" data-semantic-font="normal" data-semantic- data-semantic-parent="3" data-semantic-role="unknown" data-semantic-type="text"><mjx-c></mjx-c><mjx-c></mjx-c></mjx-mtext></mjx-mrow><mjx-script style="vertical-align: -0.15em;"><mjx-mn data-semantic-annotation="clearspeak:simple" data-semantic-font="normal" data-semantic- data-semantic-parent="3" data-semantic-role="integer" data-semantic-type="number" size="s"><mjx-c></mjx-c></mjx-mn></mjx-script></mjx-msub></mjx-mrow></mjx-script></mjx-msub></mjx-mrow></mjx-semantics></mjx-math><mjx-assistive-mml display="inline" unselectable="on"><math altimg="urn:x-wiley:26884062:media:sstr202400376:sstr202400376-math-0001" display="inline" location="graphic/sstr202400376-math-0001.png" xmlns="http://www.w3.org/1998/Math/MathML"><semantics><
二维(2D)过渡金属二掺杂物(TMDs)具有可调带隙和高载流子传输效率,因此被广泛应用于界面反应和电子器件中。然而,由于块状样品或堆叠纳米片中缺乏完全暴露的活性位点,导致其性能有限。本研究开发了一种通用方法来构建有序介孔 TMDs/金属氧化物(OM-TMDs/MOs)异质结构,包括 WS2/WO3、WSe2/WO3、WTe2/WO3、MoS2/MoO3 和 V3S4/V2O3、通过对具有有序介观结构的自组装两亲嵌段共聚物/聚氧化金属簇纳米复合材料进行一步热硫化(硒化/高纯化)。OM-TMDs/MOs 具有高度 OM 结构、高比表面积、大孔径以及异质结构框架中丰富的活性边缘位点。基于 OM-WS2/WO3 的化学电阻式气体传感器在室温下显示出优异的二氧化氮传感性能,具有高灵敏度、超高选择性(SNO2$S_{left(text{NO}right)_{2}}$/Sgas >20)和快速响应速度(6 s)。理论研究表明,WS2/WO3 异质结构和 WS2 边缘位点对 NO2 分子的强大吸附能力以及它们之间的高电荷转移有助于提高传感器的选择性和灵敏度。这种通用方法为合成基于 OM TMDs 的纳米材料提供了新的策略,在电子器件、催化、储能和转换等各种应用中显示出巨大的潜力。
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引用次数: 0
Rethinking Models of DNA Organization in Micrometer-Sized Chromosomes from the Perspective of the Nanoproperties of Chromatin Favoring a Multilayer Structure 从有利于多层结构的染色质纳米特性的角度重新思考微米级染色体中的 DNA 组织模型
Pub Date : 2024-09-04 DOI: 10.1002/sstr.202400203
Joan-Ramon Daban
The long genomic DNA molecules in eukaryotes are fragile and prone to entanglement, and must be tightly folded to fit into the micrometric dimensions of mitotic chromosomes. Histones transform the monotonous linear structure of double-helical DNA into a chromatin filament formed by many nucleosomes. A physically consistent model for the packaging of the chromatin filament must be compatible with all the constraints imposed by the structural properties of chromosomes. It has to be compatible with 1) the high concentration of DNA and the elongated cylindrical shape of chromosomes and 2) the known self-associative properties of chromatin, and also with 3) an effective protection of chromosomal DNA from topological entanglement and mechanical breakage. The multilayer chromosome model, in which a repetitive weak interaction between nucleosomes at the nanoscale produces the stacking of many chromatin layers, is compatible with all these constraints. The self-organization of the multilayer structure of the whole chromosome is consistent with current knowledge of the self-assembly of micrometric structures from different repetitive building blocks. The multilayer model justifies the geometry of chromosome bands and translocations, and is compatible with feasible physical mechanisms for the control of gene expression, and for DNA replication, repair, and segregation to daughter cells.
真核生物中的长基因组 DNA 分子非常脆弱,容易缠结,必须紧密折叠才能适应有丝分裂染色体的微米尺寸。组蛋白将双螺旋 DNA 的单线结构转化为由许多核小体形成的染色质丝。染色质丝的物理包装模型必须符合染色体结构特性所带来的所有限制。它必须符合:1)DNA 的高浓度和染色体拉长的圆柱形;2)染色质已知的自结合特性;3)有效保护染色体 DNA 免受拓扑纠缠和机械断裂。在多层染色体模型中,核小体之间在纳米尺度上的重复微弱相互作用产生了许多染色质层的堆积,这与所有这些限制条件都是一致的。整个染色体的多层结构的自组织与目前由不同重复构件自组装微观结构的知识是一致的。多层模型证明了染色体带和易位的几何形状是合理的,并与控制基因表达、DNA 复制、修复和分离到子细胞的可行物理机制相兼容。
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引用次数: 0
Directionally Cracked Mesoporous Colloidal Films by Manipulating Notch Angles and Their Anisotropic Wicking Behavior 通过调节缺口角度定向裂解介孔胶体薄膜及其各向异性的吸附行为
Pub Date : 2024-09-04 DOI: 10.1002/sstr.202400159
Yunchan Lee, Min-Gi Jo, Seongwoo Jeon, Chorong Kim, Jaekyoung Kim, Sanghyuk Wooh, Kee-Youn Yoo, Hyunsik Yoon
Wicking in porous media, such as the spreading of ink on paper or the absorption of moisture by fabric, occurs when water interacts with hydrophilic porous materials through capillary action and evaporation. The directional nature of the wicking phenomenon can be leveraged for various advanced applications, including enhanced heat transfer, colorimetric devices, energy harvesting, and microfluidics. Herein, crack generation is used to induce the anisotropic wicking of water on isolated mesoporous strips. The strips are fabricated by transforming isotropic cracks into anisotropic ones in micropyramid arrays using the Poisson effect in elastomeric blocks. Stretching an elastomeric block increases the period of a pyramid array along one direction while decreasing it in the perpendicular direction because of elastomer shrinkage. This amplifies the difference in the notch angles of pyramidal edges between parallel and perpendicular directions relative to the stretching axis. Consequently, the disparity in notch angles leads to preferential crack generation owing to elevated stress localization on the sharpened notches. Directional wicking is demonstrated using anisotropic strips of mesoporous TiO2 colloidal films and highly anisotropic wicking of ink is illustrated by coating hydrophobic films on mesoporous strips. The anisotropic wicking observed in cracked mesoporous strips can serve as 1D microfluidic channels.
当水通过毛细作用和蒸发与亲水性多孔材料相互作用时,多孔介质中的吸水现象就会发生,例如墨水在纸上的扩散或织物的吸湿。吸水现象的方向性可用于各种先进应用,包括增强传热、比色装置、能量收集和微流体技术。在这里,裂纹生成被用来诱导孤立介孔条带上水的各向异性吸水。利用弹性体块中的泊松效应,将各向同性裂缝转化为微金字塔阵列中的各向异性裂缝,从而制造出这种条带。拉伸弹性体块会增加金字塔阵列沿一个方向的周期,而由于弹性体收缩,垂直方向的周期会减少。这就扩大了金字塔边缘在平行方向和垂直方向上相对于拉伸轴线的缺口角差异。因此,切口角度的差异会导致锐化切口上的应力局部增大,从而优先产生裂纹。利用介孔二氧化钛胶体薄膜的各向异性条带演示了定向吸墨,并通过在介孔条带上涂覆疏水性薄膜说明了墨水的高度各向异性吸墨。在开裂的介孔条带中观察到的各向异性吸附可用作一维微流体通道。
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引用次数: 0
Netting Crystal Nuclei in Metal–Organic Framework Cavities 金属有机框架空腔中的网状晶核
Pub Date : 2024-09-04 DOI: 10.1002/sstr.202400300
Alan Braschinsky, Toby J. Blundell, Jonathan W. Steed
Nucleation plays an important role in crystallization outcomes, but it is still poorly understood because it occurs on short timescales and small size scales. Consequently, nucleation mechanisms are still challenging to comprehend and predict. Gaining a better understanding, and potentially control, over nucleation pathways, can significantly aid toward more consistent and targeted crystallization outcomes. To achieve this, facile methods that allow for an accurate depiction and analysis of nucleus-sized clusters are needed. Herein, the use of crystalline metal–organic frameworks (MOFs) is reported to entrap clusters of small organic molecules, allowing for an accurate representation of the size and shape of the confined clusters via single-crystal X-Ray diffraction analysis. This is realized by synthesizing high-quality single crystals of lanthanum-based MOFs, which provides well-defined pore spaces for the encapsulation of guest molecules. The results show that the size and shape of the guest molecular clusters within MOFs significantly differ from their bulk equivalents, suggesting that this method can also be used toward discovering novel polymorphs. Additionally, the findings indicate that these small molecular clusters form via intermolecular interactions that do not always dominate the bulk packing, shedding new light on the initial molecular aggregation mechanisms of precritical nuclei.
成核在结晶结果中发挥着重要作用,但由于其发生的时间尺度短、尺寸尺度小,人们对它的了解还很不够。因此,成核机制的理解和预测仍然具有挑战性。更好地了解并控制成核途径,可大大有助于实现更一致、更有针对性的结晶结果。要实现这一目标,需要能够准确描绘和分析晶核大小晶簇的简便方法。本文报告了利用结晶金属有机框架(MOFs)来捕获小分子有机物簇,从而通过单晶 X 射线衍射分析来准确呈现受限簇的大小和形状。这是通过合成高质量的镧基 MOFs 单晶实现的,这种单晶为客体分子的封装提供了定义明确的孔隙。研究结果表明,MOFs 中客体分子团簇的大小和形状与块状分子团簇明显不同,这表明这种方法也可用于发现新型多晶体。此外,研究结果表明,这些小分子团簇是通过分子间相互作用形成的,而这种相互作用并不总是在团状填料中占主导地位,从而为预临界核的初始分子聚集机制提供了新的思路。
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引用次数: 0
Tracking Water Splitting Activity by Cocatalyst Identity in SrTiO3 通过 SrTiO3 中催化剂的特性跟踪水分离活性
Pub Date : 2024-09-04 DOI: 10.1002/sstr.202400283
Nursaya Zhumabay, Jeremy A. Bau, Rafia Ahmad, Laurentiu Braic, Huabin Zhang, Luigi Cavallo, Magnus Rueping
Photocatalytic water splitting is the most idealistic route to green hydrogen production, but the extensive material requirements for this reaction make it difficult to realize good photocatalysts. Noble metal cocatalysts are often added to photocatalysts to aid in charge separation and improve surface kinetics for H2 evolution. Herein, the high activity of the promising photocatalyst Al-doped SrTiO3 is demonstrated to be ultimately dependent on the cocatalyst used as much as the presence of Al dopant. By tracking the band energetics of photocatalyst electrodes using operando electrochemical attenuated total reflectance surface-enhanced infrared absorption spectroscopy, cocatalysts (especially Rh) are found to shift the quasi-Fermi levels and metal-semiconductor flat-band potentials of photocatalysts in an anodic direction. Furthermore, the size of the shift directly correlates with overall water splitting activity, demonstrating that SrTiO3 becomes more active as photogenerated electrons are stabilized further from the conduction band. Rh on Al-doped SrTiO3 provides the most advantageous band tailoring as confirmed by density functional theory and is experimentally found to provide this effect by eliminating Ti3+-related surface traps in the presence of Al dopants. Therefore, the effect of cocatalysts on water splitting activity is more complicated than previously thought.
光催化水分裂是最理想的绿色制氢途径,但这一反应对材料的要求很高,因此很难实现良好的光催化剂。贵金属茧催化剂通常被添加到光催化剂中,以帮助电荷分离并改善氢进化的表面动力学。在这里,有前途的掺铝 SrTiO3 光催化剂的高活性最终取决于所使用的助催化剂以及 Al 掺杂的存在。通过使用操作电化学衰减全反射表面增强红外吸收光谱跟踪光催化剂电极的带能,发现共催化剂(尤其是 Rh)会使光催化剂的准费米级和金属半导体平带电位向阳极方向移动。此外,偏移的大小与整体水分离活性直接相关,这表明随着光生电子进一步从导带稳定下来,SrTiO3 的活性会越来越高。密度泛函理论证实,铝掺杂的 SrTiO3 上的 Rh 提供了最有利的带定制,实验发现,在铝掺杂存在的情况下,Rh 通过消除与 Ti3+ 相关的表面陷阱提供了这种效果。因此,共催化剂对水分离活性的影响比以前想象的要复杂得多。
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引用次数: 0
Double Anthracene-Based Sensitizers for High-Efficiency Dye-Sensitized Solar Cells under Both Sunlight and Indoor Light 日光和室内光下高效染料敏化太阳能电池的双蒽基敏化剂
Pub Date : 2024-09-04 DOI: 10.1002/sstr.202400236
Faraghally A. Faraghally, Ahmed Fouad Musa, Ching-Chin Chen, Yu-Hsuan Chen, Yan-Da Chen, Chen-Yu Yeh, Tzu-Chien Wei
The development of photosensitizers with extended π-conjugation and spectral matching to sunlight and fluorescent light is crucial for achieving high power conversion efficiency (PCE) in dye-sensitized solar cells (DSSCs). This study presents a series of novel anthracene-based photosensitizers, AMO1–AMO4. This series has been designed with bulky modified Hagfeldt donors to suppress undesired molecular aggregation, double anthracene groups for enhanced π-conjugation, acetylene groups for improved molecular planarity, and four distinct acceptors to fine-tune their photophysical and electrochemical properties. The performance of the novel dyes in DSSCs is investigated using two copper redox shuttles, CuI/II(dmp)2 and CuI/II(dmodmbp)2. Among the investigated dyes, AMO2 mediated with CuI/II(dmodmbp)2 exhibits the highest power conversion efficiency (PCE) of 10.05% (JSC = 13.72 mA cm 2, VOC = 1.035 V, and FF = 0.71) under sunlight illumination and an outstanding PCE of 34.64% under T5 illumination (6000 lux). These achievements underscore the remarkable potential of anthracene-bridged sensitized DSSCs in indoor and outdoor applications.
要在染料敏化太阳能电池(DSSC)中实现高功率转换效率(PCE),开发具有扩展π共轭和光谱匹配太阳光和荧光的光敏剂至关重要。本研究介绍了一系列新型蒽基光敏剂 AMO1-AMO4。设计该系列染料时,使用了大块修饰的哈格菲尔德供体以抑制不希望的分子聚集,使用了双蒽基团以增强π共轭,使用了乙炔基团以改善分子平面性,还使用了四种不同的受体以微调其光物理性质和电化学性质。利用两种铜氧化还原梭子--CuI/II(dmp)2 和 CuI/II(dmodmbp)2,研究了新型染料在 DSSC 中的性能。在所研究的染料中,CuI/II(dmodmbp)2 介导的 AMO2 在日光照明下的功率转换效率(PCE)最高,达到 10.05%(JSC = 13.72 mA cm 2,VOC = 1.035 V,FF = 0.71),而在 T5 照明(6000 勒克斯)下的 PCE 则高达 34.64%。这些成就凸显了蒽桥敏化 DSSC 在室内和室外应用中的巨大潜力。
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引用次数: 0
Tuning Surface Chemistry in 2D Layered BiOI by Facile Liquid-Phase Exfoliation for Enhanced Photoelectrocatalytic Oxygen Evolution 通过便捷的液相剥离技术调节二维层状生物氧化物的表面化学性质,从而增强光电催化氧进化能力
Pub Date : 2024-09-04 DOI: 10.1002/sstr.202400275
Mengjiao Wang, Jaime Gallego, Micaela Pozzati, Teresa Gatti
BiOI is a promising photoelectrocatalyst for oxidation reactions. However, the limited photoelectrocatalytic (PEC) activity necessitates the development of new strategies to modify its surface chemistry and thus enhance functional properties. Herein, we present a simple method to increase photocurrent in a BiOI-based photoanode by exfoliating microspheres of the oxyhalide produced through hydrothermal synthesis. Following exfoliation in isopropanol, the resulting layered BiOI-based colloid contains a greater variety of species, including Bi2O2CO3, I3, IO3, Bi5+, and hydroxides, compared to the original BiOI. These additional species do not directly enhance the PEC oxygen evolution reaction (OER) performance. Instead, they are consumed or converted during PEC OER, resulting in more active sites on the photoelectrode and reduced resistance, which ultimately improves the water oxidation performance of the exfoliated BiOI. Over long-term chronoamperometry, the exfoliated BiOI demonstrates a photocurrent twice as high as that of the BiOI microspheres. Analysis of the species after PEC OER reveals that the combination of IO3, Bi5+, and I3 species on the BiOI is beneficial for charge transfer, thus enhancing the intrinsic PEC properties of the BiOI. This study offers new insights into the role of surface chemistry in determining PEC performance, aiding the optimization of 2D materials-based photoelectrocatalysts.
BiOI 是一种用于氧化反应的前景广阔的光电催化剂。然而,由于其光电催化(PEC)活性有限,因此有必要开发新的策略来改变其表面化学性质,从而增强其功能特性。在此,我们提出了一种简单的方法,通过剥离水热合成产生的氧卤化物微球,提高基于 BiOI 的光阳极的光电流。在异丙醇中剥离后,与原始 BiOI 相比,生成的层状 BiOI 基胶体含有更多种类,包括 Bi2O2CO3、I3-、IO3-、Bi5+ 和氢氧化物。这些额外的物种不会直接提高 PEC 氧进化反应(OER)的性能。相反,它们会在 PEC 氧进化反应过程中被消耗或转化,从而在光电极上形成更多的活性位点并降低电阻,最终提高剥离的 BiOI 的水氧化性能。在长期的计时器测量中,剥离的生物氧化物的光电流是生物氧化物微球的两倍。对 PEC OER 后的物种分析表明,BiOI 上 IO3-、Bi5+ 和 I3- 物种的组合有利于电荷转移,从而增强了 BiOI 的内在 PEC 特性。这项研究为了解表面化学在决定 PEC 性能方面的作用提供了新的视角,有助于优化基于二维材料的光电催化剂。
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引用次数: 0
pH-Sensitive Magnetic Nanoparticle-Mediated Natural-Killer-Cell-Based Microrobots for Dual-Targeted Delivery and Induction of Pro-Inflammatory Macrophage Polarization pH值敏感的磁性纳米粒子介导的天然杀伤细胞微机器人可实现双重靶向递送和诱导促炎性巨噬细胞极化
Pub Date : 2024-09-02 DOI: 10.1002/sstr.202400149
Van Du Nguyen, Jieun Park, Seoyeon Choi, Kim Tien Nguyen, Hyungwoo Kim, Jong-Oh Park, Eunpyo Choi
Adoptive cell therapy using natural killer (NK) cells emerges as the next-generation cancer immunotherapy. Based on the intrinsic capability of direct cancer cell necrosis without prior education, a chemotherapeutic, free-drug delivery, NK-cell-based platform can be developed. However, weak targeting of NK cells to solid tumors is observed. In addition, to boost the tumor-killing efficiency, another immune-regulating function should be added to the cells. Herein, a NK-cell-based hybrid system (NK-Robot) conjugated with magnetic nanoparticles (MNPs) that provides 1) efficient guidance of NK cells and 2) targeted delivery of MNPs in situ is demonstrated, taking advantage of a newly designed, stimuli-responsive polymeric linker. Thus, NK cells are allowed to target tumors under magnetic control conditions, and the liberated MNPs effectively reeducate the tumor-associated macrophages (M2) to antitumor macrophages (M1), beneficial for the immunotherapy of tumors. In vivo experiments on BALB/c nude mice further support the finding that NK-Robots effectively inhibit tumor growth.
使用自然杀伤(NK)细胞的适应性细胞疗法已成为下一代癌症免疫疗法。基于 NK 细胞无需事先教育即可直接杀死癌细胞的内在能力,可以开发出一种基于 NK 细胞的化疗、自由给药平台。然而,NK 细胞对实体瘤的靶向性较弱。此外,要想提高杀灭肿瘤的效率,还需要在细胞中加入另一种免疫调节功能。本文展示了一种基于 NK 细胞的混合系统(NK-Robot),该系统与磁性纳米粒子(MNPs)连接,利用新设计的刺激响应型聚合物连接体,可提供:1)NK 细胞的高效引导;2)MNPs 的原位靶向递送。这样,NK 细胞就能在磁控制条件下靶向肿瘤,而释放的 MNPs 能有效地将肿瘤相关巨噬细胞(M2)再教育为抗肿瘤巨噬细胞(M1),从而有利于肿瘤的免疫治疗。在 BALB/c 裸鼠身上进行的体内实验进一步证实了 NK-Robots 能有效抑制肿瘤生长的结论。
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引用次数: 0
Decoupling Volatile and Nonvolatile Response in Reliable Halide Perovskite Memristors 可靠的卤化物包光体晶闸管中挥发性和非挥发性响应的解耦
Pub Date : 2024-08-29 DOI: 10.1002/sstr.202400380
Naresh-Kumar Pendyala, Cedric Gonzales, Antonio Guerrero
Halide perovskite is very attractive for the fabrication of energy-efficient memristors for neuromorphic applications. However, reproducibility, stability, and understanding the switching behavior still lag in comparison to other technologies. Herein, a deep-level understanding of perovskite memristors is obtained by the development of highly reproducible devices. The approach is based on a highly stable perovskite formulation (MAPbBr3) and the use of preoxidized silver (AgI) as a buffer layer. Here, reliable perovskite memristors with device yields approaching 100%, stabilities of >104 cycles for volatile response, and adequate conditions for linear potentiation/depression for nonvolatile response are demonstrated. Using these devices, the nature of the dual volatile and nonvolatile response is understood. It is shown that applying short SET voltage (VSET) pulses leads to ion displacement inside the perovskite material with the formation of an ionic double layer close to the contacts. The displacement of the ions contributes to the series resistance of the device and to a volatile response with ions diffusing back to the perovskite at V < VSET. Alternatively, long VSET pulses lead to a gradual increase in current, the appearance of a chemical inductor, and a nonvolatile response. The observed nonvolatile regime is related to the formation of Ag+ conductive filaments.
卤化物包晶对于制造用于神经形态应用的高能效忆阻器极具吸引力。然而,与其他技术相比,可重复性、稳定性和对开关行为的理解仍然落后。在本文中,通过开发高度可重现的器件,我们对包晶体忆阻器有了深层次的了解。该方法基于一种高度稳定的过氧化物配方(MAPbBr3),并使用预氧化银(AgI)作为缓冲层。在这里,我们展示了可靠的过氧化物忆阻器,其器件产量接近 100%,挥发性响应的稳定性达到 104 个周期,非挥发性响应的线性增效/抑制条件充分。通过使用这些器件,我们了解了易失性和非易失性双响应的性质。研究表明,施加短 SET 电压(VSET)脉冲会导致过氧化物材料内部的离子位移,并在触点附近形成离子双层。离子的位移会增加器件的串联电阻,并导致离子在 V < VSET 时扩散回包晶的波动响应。另一种情况是,长 VSET 脉冲导致电流逐渐增加,出现化学感应和非挥发性响应。观察到的非挥发性机制与 Ag+ 导电丝的形成有关。
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引用次数: 0
Ultrahigh Breakdown Field in Gallium (III) Oxide Dielectric Structure Fabricated by Novel Aerosol Deposition Method 用新型气溶胶沉积法制造的氧化镓(III)电介质结构中的超高击穿场强
Pub Date : 2024-08-21 DOI: 10.1002/sstr.202400321
Jun-Woo Lee, Jong Ho Won, Woosup Kim, Jwa-Bin Jeon, Myung-Yeon Cho, Sunghoon Kim, Minkyung Kim, Chulhwan Park, Weon Ho Shin, Kanghee Won, Sang-Mo Koo, Jong-Min Oh
With the increasing demand for modern high-voltage electronic devices in electric vehicles and renewable-energy systems, power semiconductor devices with high breakdown fields are becoming essential. β-Gallium oxide (Ga2O3), which has a theoretical breakdown field of 8 MV cm−1, is being studied as a next-generation power-switch material. However, realizing a breakdown field close to this theoretical value remains challenging. In this study, an aerosol deposition-manufactured Ga2O3 film boasting an extremely high breakdown field, achieved through thickness optimization, heat treatment, and a unique nozzle-tilting method, is developed. This study explores the effect of oxygen vacancies on the dielectric constant, breakdown field, and microstructure of Ga2O3 films. Through these methods, Ga2O3 films with a denser (98.88%) and uniform surface, made less affected by oxygen vacancies through nozzle tilting and post-annealing at 800 °C, are produced, resulting in appropriate dielectric constants (9.3 at 10 kHz), low leakage currents (5.8 × 10−11 A cm−2 at 20 kV cm−1), and a very high breakdown field of 5.5 MV cm−1. The results of this study suggest that aerosol-deposited Ga2O3 layers have great potential to enable power switches with reliable switching.
随着电动汽车和可再生能源系统对现代高压电子设备的需求日益增长,具有高击穿场的功率半导体器件变得至关重要。β-氧化镓(Ga2O3)的理论击穿场强为 8 MV cm-1,目前正被作为下一代功率开关材料进行研究。然而,实现接近这一理论值的击穿场仍然具有挑战性。本研究开发了一种气溶胶沉积制造的 Ga2O3 薄膜,通过厚度优化、热处理和独特的喷嘴倾斜方法实现了极高的击穿场强。本研究探讨了氧空位对 Ga2O3 薄膜介电常数、击穿场和微观结构的影响。通过这些方法,生产出了表面致密(98.88%)且均匀的 Ga2O3 薄膜,通过喷嘴倾斜和在 800 °C 下进行后退火,减少了氧空位的影响,从而获得了适当的介电常数(10 kHz 时为 9.3)、低漏电流(20 kV cm-1 时为 5.8 × 10-11 A cm-2)和 5.5 MV cm-1 的极高击穿场。研究结果表明,气溶胶沉积 Ga2O3 层在实现可靠开关的功率开关方面具有巨大潜力。
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