heterojunctions

异质结
  • 文章类型: Journal Article
    使用2D原子晶体及其异质结构进行类脑计算,通过模仿人类大脑在信息处理中的显着效率和最小的能耗,为vonNeumann架构中固有的能效和处理速度限制提供了一个强大的解决方案。然而,传统的2D材料为基础的异质结构在脑样装置中采用的是有局限性的,性能均匀性,制造错综复杂,和弱的界面附着力,这限制了它们更广泛的应用。新型二维原子-分子异质结(2DAMH)的引入,通过2D材料与功能分子的共价官能化实现,通过提供功能的稳定性和可调性,为类似大脑的设备开创了一个新时代。这篇综述主要探讨了2DAMH的电子属性,该属性源自聚合物材料与2D材料的协同作用,强调它们在忆阻器件中的利用的最新进展,特别是它们在复制生物突触功能方面的潜力。尽管在修改的精确性方面一直存在挑战,生产中的可扩展性,以及基础理论的完善,创新研究的激增正在积极寻求解决方案。这些努力阐明了将2DAMH纳入大脑启发的智能系统的巨大潜力,强调实现更高效和节能的计算范例的前景。
    Brainoid computing using 2D atomic crystals and their heterostructures, by emulating the human brain\'s remarkable efficiency and minimal energy consumption in information processing, poses a formidable solution to the energy-efficiency and processing speed constraints inherent in the von Neumann architecture. However, conventional 2D material based heterostructures employed in brainoid devices are beset with limitations, performance uniformity, fabrication intricacies, and weak interfacial adhesion, which restrain their broader application. The introduction of novel 2D atomic-molecular heterojunctions (2DAMH), achieved through covalent functionalization of 2D materials with functional molecules, ushers in a new era for brain-like devices by providing both stability and tunability of functionalities. This review chiefly delves into the electronic attributes of 2DAMH derived from the synergy of polymer materials with 2D materials, emphasizing the most recent advancements in their utilization within memristive devices, particularly their potential in replicating the functionality of biological synapses. Despite ongoing challenges pertaining to precision in modification, scalability in production, and the refinement of underlying theories, the proliferation of innovative research is actively pursuing solutions. These endeavors illuminate the vast potential for incorporating 2DAMH within brain-inspired intelligent systems, highlighting the prospect of achieving a more efficient and energy-conserving computing paradigm.
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  • 文章类型: Journal Article
    钙钛矿直接X射线探测器的开发显示出提高医学成像和工业检测精度的潜力。为了确保X射线的最佳能量转换效率,以降低辐射剂量,需要使用厚度达到几百微米甚至几毫米的钙钛矿。然而,非线性电流响应变得不确定与这样的高厚度。例如,关于浅层缺陷快速捕获和释放电荷的普遍理论不足以解释在高质量单晶样品中观察到的非线性电流响应。此外,显著的非线性电流响应会降低检测性能。这里,我们阐明了钙钛矿中特殊的寄生和漂移电容引起的非线性电流响应,除了浅层缺陷外,还由于体结构缺陷和界面结宽度变化而引起。理论分析和实验结果均表明,通过建立本体异质结和细化界面结,可以有效抑制非线性电流响应。因此,我们已经成功开发了基于多晶MAPbI3厚膜的高度线性电流响应检测器。值得注意的是,这些探测器在100kVpX射线辐照下以0.1V/μm的低偏压实现了2.3×104μC·Gyair-1·cm-2的记录灵敏度,为高密度物体提供持久和高分辨率的X射线成像。64×64像素平板原型探测器的成功制造和测试证实了这些策略在校正基于钙钛矿的X射线探测器中的非线性电流响应方面的广泛适用性。
    The development of perovskite direct X-ray detectors shows potential for advancing medical imaging and industrial inspection precision. To ensure the optimal energy conversion efficiency of X-rays for reducing radiation doses, it is necessary for perovskites with thicknesses reaching hundreds of micrometers or even several millimeters to be utilized. However, the nonlinear current response becomes uncertain with such high thicknesses. For instance, the prevailing theory regarding the rapid trapping and release of charges by shallow-level defects falls short in explaining the nonlinear current response observed in high-quality single-crystal samples. Moreover, a significant nonlinear current response can degrade the detection performance. Here, we elucidate peculiar parasitic and drift capacitance-induced nonlinear current responses in perovskites, which arise from bulk structural deficiencies and interface junction width variation in addition to shallow-level defects. Both theoretical analysis and experimental findings demonstrate the effective suppression of nonlinear current responses by establishing bulk heterojunctions and refining interface junctions. Consequently, we have successfully developed highly linear current-responsive detectors based on polycrystalline MAPbI3 thick films. Notably, these detectors achieve a record sensitivity of 2.3 × 104 μC·Gyair-1·cm-2 under 100 kVp X-ray irradiation with a low bias of 0.1 V/μm, enabling enduring and high-resolution X-ray imaging for high-density objects. Successful fabrication and testing of a 64 × 64-pixel flat-panel prototype detector affirm the widespread applicability of these strategies in rectifying nonlinear current responses in perovskite-based X-ray detectors.
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  • 文章类型: Journal Article
    回顾两种不同半导体或半导体与金属之间形成异质结的成熟理论,可以阐明热催化中使用的纳米杂化系统的显着催化性能。在产生异质结时,涉及纳米颗粒或纳米尺寸的薄膜,由于它们的尺寸,可能会完全充满耗尽或积累区域发展产生的空间电荷。这种现象决定了催化位点的性质,并因此影响了这种纳米杂化物的催化活性。以下观点提出了这一概念和实验结果的例子,证实了它的有效性,加上一个非常有效的工具,冷等离子体沉积,用于以受控方式设计和实现具有异质结的纳米杂化结构。这种方法无疑将拓宽当代纳米催化剂“炼金术”的视野。
    Recalling the well-established theory of heterojunction formation between two different semiconductors or a semiconductor and a metal can elucidate the remarkable catalytic properties of nanohybrid systems employed in thermal catalysis. Upon the creation of heterojunctions, involved nanoparticles or nanometer-sized thin films, as a result of their dimensions, may become entirely filled with space charges generated from the development of depletion or accumulation regions. This phenomenon dictates the nature of catalytic sites and consequently affects the catalytic activity of such nanohybrids. The following perspective presents this concept and examples of experimental results that substantiate its validity, along with an extremely effective tool, cold plasma deposition, for designing and realizing in a controlled manner the structure of nanohybrids with heterojunctions. This approach will undoubtedly broaden the view of the contemporary \"alchemy\" of nanocatalysts.
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  • 文章类型: Journal Article
    光催化制氢提供了建立可持续能源经济的替代途径。虽然许多光敏材料显示出从水中产生氢的潜力,通过以异质结形式结合具有互补性质的两种不同材料所实现的协同作用可以显著地实现它们的光催化活性。我们的研究描述了由RuO2/N组成的金属-有机骨架衍生(MOF)金属氧化物异质结的设计和生成,S-TiO2。RuO2/N,S-TiO2是通过MOFs的热解产生的,Ru-HKUST-1和氨基官能化的MIL-125-NH2。在各种RuO2/N中,S-TiO2材料测试,以最低RuO2含量为特征的材料,表现出最高的氢析出速率,在纯水中产生10,761μmol·hr-1·g-1的氢,表观量子产率为10.0%。除了RuO2/N,S-TiO2,我们产生了另外两个MOF衍生的金属氧化物异质结,ZnO/N,S-TiO2和In2O3/N,S-TiO2,导致0.7%和0.3%的表观量子产率,分别。在RuO2/N中观察到显著的光催化活性,S-TiO2被认为是由于金属氧化物固有的金属性能的组合产生的协同效应,他们的乐队对齐,孔隙度,和从父MOF继承的曲面属性。RuO2/N的光催化效率,S-TiO2在实际水样中得到了进一步证明,在自来水中以8,190μmol·hr-1·g-1的速率生产氢气。
    Photocatalytic hydrogen production offers an alternative pathway to establish a sustainable energy economy. While numerous photoactive materials exhibit potential for generating hydrogen from water, the synergy achieved by combining two different materials with complementary properties in the form of heterojunctions can significantly their photocatalytic activity. Our study describes the design and generation of the metal-organic framework-derived (MOF) metal oxide heterojunction composed of RuO2/N,S-TiO2. The RuO2/N,S-TiO2 is generated through the pyrolysis of MOFs, Ru- HKUST-1, and the amino-functionalized MIL-125-NH2. Among the various RuO2/N,S- TiO2 materials tested, the material characterized by the lowest RuO2 content, exhibited the highest hydrogen evolution rate, producing 10,761 μmol·hr-1·g-1 of hydrogen with an apparent quantum-yield of 10.0% in pure water. In addition to RuO2/N,S-TiO2, we generated two other MOF-derived metal-oxide heterojunctions, ZnO/N,S-TiO2 and In2O3/N,S-TiO2, leading to apparent quantum yields of 0.7% and 0.3%, respectively. The remarkable photocatalytic activity observed in RuO2/N,S-TiO2 is thought to be attributed to the synergistic effects arising from the combination of metallic properties inherent in the metal oxides, their band alignment, porosity, and surface properties inherited from the parent MOFs. The photocatalytic efficiency of RuO2/N,S-TiO2 was further demonstrated in actual water samples, producing hydrogen with a rate of 8,190 μmol·hr-1·g-1 in tap water.
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  • 文章类型: Journal Article
    构建独特的异质结构是增强过渡金属硒化物的K存储能力的高效方法。这种结构产生显著降低电荷转移活化能的内部电场。然而,实现保持最佳能级梯度和晶格匹配程度的完美界面区域仍然是一个相当大的挑战。在这项研究中,我们合成了Setaria样NiTe2/MoS2@C异质界面,在该界面上,三维MoS2纳米片均匀地嵌入NiTe2纳米棒中以形成稳定的异质结。NiTe2/MoS2异质结由于其低晶格失配(δ=13%)而显示出独特的电子构型和几个活性位点。强电场,和均匀的碳壳。钾离子电池(KIB)中的NiTe2/MoS2@C阳极在500mAg-1的速率下进行1000次循环后表现出令人印象深刻的可逆容量为125.8mAh/g,并且即使在1000mAg-1的3000次循环后仍具有111.7mAh/g的稳定可逆容量。甚至NiTe2/MoS2@C//四羧酸二酐全电池配置在200mAg-1下100次循环后仍保持了92.4mAh/g的显着可逆容量,突显了其在KIB中的应用潜力。计算进一步表明,精心设计的NiTe2/MoS2异质结显着促进K离子扩散。
    Constructing unique heterostructures is a highly effective approach for enhancing the K+ storage capability of transition metal selenides. Such structures generate internal electric fields that significantly reduce the charge transfer activation energy. However, achieving a flawless interfacial region that maintains the optimal energy level gradient and degree of lattice matching remains a considerable challenge. In this study, we synthesised Setaria-like NiTe2/MoS2@C heterogeneous interfaces at which three-dimensional MoS2 nanosheets are evenly embedded in NiTe2 nanorods to form stabilised heterojunctions. The NiTe2/MoS2 heterojunctions display distinctive electronic configurations and several active sites owing to their low lattice misfits (δ = 13 %), strong electric fields, and uniform carbon shells. A NiTe2/MoS2@C anode in a potassium-ion battery (KIB) exhibited an impressive reversible capacity of 125.8 mAh/g after 1000 cycles at a rate of 500 mA g-1 and a stable reversible capacity of 111.7 mAh/g even after 3000 cycles at 1000 mA g-1. Even the NiTe2/MoS2@C//perylene tetracarboxylic dianhydride full battery configuration maintained a significant reversible capacity of 92.4 mAh/g after 100 cycles at 200 mA g-1, highlighting its considerable potential for application in KIBs. Calculations further revealed that the well-designed NiTe2/MoS2 heterojunction significantly promotes K+ ion diffusion.
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  • 文章类型: Journal Article
    在这项研究中,我们报告了在室温下基于二硒化钼-氧化锌异质结装饰rGO(MoSe2/ZnO/rGO)的三元纳米复合材料的增强传感响应乙醇气体传感装置。已针对各种浓度的乙醇气体(1-500ppm)分析了三元纳米复合材料传感装置的传感性能。气体传感结果表明,对于500ppm乙醇气体浓度,感测装置表现出50.2的增强的响应值(Rg/Ra)。重要的是,感应装置的快速响应和恢复时间分别为6.2s和12.9s。除此之外,该传感装置对乙醇气体的长期检测(45天)显示出了巨大的前景。该传感装置已经证明了在Ippm的非常低的浓度下检测乙醇的能力。三元纳米复合传感器件的增强传感性能凸显了MoSe2纳米片之间的有效协同作用,ZnO纳米棒,和rGO纳米片。这归因于三元纳米复合传感器中两个异质结的形成:MoSe2和ZnO之间的p-n异质结以及MoSe2和rGO之间的p-p异质结。对结果的分析表明,提出的MoSe2/ZnO/rGO纳米复合传感装置可以被认为是实时检测乙醇气体的有希望的候选者。
    In this research, we report an enhanced sensing response ethanol gas sensing device based on a ternary nanocomposite of molybdenum diselenide-zinc oxide heterojunctions decorated rGO (MoSe2/ZnO/rGO) at room temperature. The sensing performance of the ternary nanocomposite sensing device has been analysed for various concentrations of ethanol gas (1-500 ppm). The gas-sensing results have revealed that for 500 ppm ethanol gas concentration, the sensing device has exhibited an enhanced response value(Rg/Ra)of 50.2. Significantly, the sensing device has displayed a quick response and recovery time of 6.2 and 12.9 s respectively. In addition to this, the sensing device has shown a great prospect for long-term detection of ethanol gas (45 days). The sensing device has demonstrated the ability to detect ethanol at remarkably low concentrations of 1 ppm. The enhanced sensing performance of the ternary nanocomposite sensing device has highlighted the effective synergistic effect between MoSe2nanosheets, ZnO nanorods, and rGO nanosheets. This has been attributed to the formation of two heterojunctions in the ternary nanocomposite sensor: a p-n heterojunction between MoSe2and ZnO and a p-p heterojunction between MoSe2and rGO. The analysis of the results has suggested that the proposed MoSe2/ZnO/rGO nanocomposite sensing device could be considered a promising candidate for the real-time detection of ethanol gas.
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  • 文章类型: Journal Article
    基于过渡金属二硫属化合物(TMD)的范德华异质结提供了操纵发光和光捕获行为的高级策略。决定光材料相互作用的关键因素是异质结界面处的能带排列,特别是I型和II型比对之间的区别。然而,在不改变组成材料的情况下将带对准从一种类型改变到另一种类型是异常困难的。这里,利用具有厚度依赖性带隙的Bi2O2Se作为底层,我们提出了一种创新策略,用于在WS2/Bi2O2Se异质结中设计界面带配置。特别是,通过将Bi2O2Se底层的厚度从单层增加到多层,我们实现了从I型(Bi2O2Se跨越WS2)到II型,最后到I型(WS2跨越Bi2O2Se)的能带排列的调谐。我们使用稳态和瞬态光谱以及密度泛函理论计算验证了这种带结构转换。使用这种材料组合,我们进一步设计了一个包含I型(WS2跨Bi2O2Se,荧光猝灭)和I型(Bi2SeO5跨骑WS2,荧光恢复)通过聚焦激光束(FLB)在一个样品中对齐。通过对FLB轨迹进行编程,我们在WS2上实现了预先设计的局部荧光微图案,而不改变其内在原子结构。这种有效的带结构设计策略代表了利用TMD异质结用于多功能光子应用的潜力的重大飞跃。
    van der Waals heterojunctions based on transition-metal dichalcogenides (TMDs) offer advanced strategies for manipulating light-emitting and light-harvesting behaviors. A crucial factor determining the light-material interaction is in the band alignment at the heterojunction interface, particularly the distinctions between type-I and type-II alignments. However, altering the band alignment from one type to another without changing the constituent materials is exceptionally difficult. Here, utilizing Bi2O2Se with a thickness-dependent band gap as a bottom layer, we present an innovative strategy for engineering interfacial band configurations in WS2/Bi2O2Se heterojunctions. In particular, we achieve tuning of the band alignment from type-I (Bi2O2Se straddling WS2) to type-II and finally to type-I (WS2 straddling Bi2O2Se) by increasing the thickness of the Bi2O2Se bottom layer from monolayer to multilayer. We verified this band architecture conversion using steady-state and transient spectroscopy as well as density functional theory calculations. Using this material combination, we further design a sophisticated band architecture incorporating both type-I (WS2 straddles Bi2O2Se, fluorescence-quenched) and type-I (Bi2SeO5 straddles WS2, fluorescence-recovered) alignments in one sample through focused laser beam (FLB). By programming the FLB trajectory, we achieve a predesigned localized fluorescence micropattern on WS2 without changing its intrinsic atomic structure. This effective band architecture design strategy represents a significant leap forward in harnessing the potential of TMD heterojunctions for multifunctional photonic applications.
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  • 文章类型: Journal Article
    视网膜启发的视觉传感器在神经形态视觉系统的实现中起着至关重要的作用。然而,在光刺激的背景下,追求实现双向突触行为和获得高性能的过程中仍然存在重大障碍。在这项研究中,我们提出了一种基于IGZO/SnO/SnS异质结构的可重构全光控制突触装置,集成了传感,存储和处理功能。依靠简单的异质结堆叠结构和能带工程的作用,在紫外线(266nm)和可见光(405、520和658nm)的光刺激下,可以观察到突触的兴奋和抑制行为,而无需额外的电压调制。特别是,制造了基于IGZO/SnO/SnS异质结构的结型场效应晶体管,以阐明潜在的双向光响应机制。除了光信号处理,对基于光电突触的人工神经网络模拟器进行了训练和识别,识别率为91%。此外,我们制备了一个8×8的光电突触阵列,并成功地演示了人脑图像识别的感知和记忆过程,以及模拟紫外线对视网膜的损伤情况。这项工作为开发高性能的全光学控制的光电突触提供了有效的策略,并为多功能人工神经网络视觉系统的设计提供了实用的方法。
    Retina-inspired visual sensors play a crucial role in the realization of neuromorphic visual systems. Nevertheless, significant obstacles persist in the pursuit of achieving bidirectional synaptic behavior and attaining high performance in the context of photostimulation. In this study, we propose a reconfigurable all-optical controlled synaptic device based on the IGZO/SnO/SnS heterostructure, which integrates sensing, storage and processing functions. Relying on the simple heterojunction stack structure and the role of energy band engineering, synaptic excitatory and inhibitory behaviors can be observed under the light stimulation of ultraviolet (266 nm) and visible light (405, 520 and 658 nm) without additional voltage modulation. In particular, junction field-effect transistors based on the IGZO/SnO/SnS heterostructure were fabricated to elucidate the underlying bidirectional photoresponse mechanism. In addition to optical signal processing, an artificial neural network simulator based on the optoelectrical synapse was trained and recognized handwritten numerals with a recognition rate of 91%. Furthermore, we prepared an 8 × 8 optoelectrical synaptic array and successfully demonstrated the process of perception and memory for image recognition in the human brain, as well as simulated the situation of damage to the retina by ultraviolet light. This work provides an effective strategy for the development of high-performance all-optical controlled optoelectronic synapses and a practical approach to the design of multifunctional artificial neural vision systems.
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  • 文章类型: Journal Article
    混合DFT计算用于比较Cu的吸附和稳定,Ag,和Au原子在石墨C3N4上以及由g-C3N4和TiO2形成的异质结上。虽然Cu和Ag可以以阳离子的形式强烈地化学吸附在g-C3N4上,但Au仅微弱地物理吸附。在g-C3N4/TiO2上,所有硬币金属吸附原子都可以被强化学吸附,但是,当Cu和Ag形成阳离子时,Au形成Au种。从头算分子动力学模拟证实,g-C3N4上的金属原子在室温下具有高度的流动性,虽然它们仍然限制在异质结上C3N4和TiO2之间的界面间距中,在催化循环中对反应物既稳定结合又可到达。因此,用金属单原子掺杂g-C3N4/TiO2允许产生具有可调电荷和化学性质并且相对于裸C3N4具有改善的稳定性的催化体系。此外,金属单原子的存在引起的g-C3N4/TiO2电子结构的变化也有利于光催化应用。
    Hybrid DFT calculations are employed to compare the adsorption and stabilization of Cu, Ag, and Au atoms on graphitic C3N4 and on the heterojunction formed by g- C3N4 and TiO2. While Cu and Ag can be strongly chemisorbed in form of cations on g- C3N4, Au is only weakly physisorbed. On g- C3N4/TiO2, all coinage metal adatoms can be strongly chemisorbed, but, while Cu and Ag forms cations, Au form an Au- species. Ab Initio Molecular Dynamics simulations confirm that the metal adatoms on g-C3N4 are highly mobile at room temperature, while they remain confined in the interfacial spacing between C3N4 and TiO2 on the heterojunction, being both stably bound and reachable for the reactants in a catalytic cycle. Doping g- C3N4/TiO2 with metal single atoms permits thus to generate catalytic systems with tunable charge and chemical properties and improved stability with respect to bare C3N4. Moreover, the changes in the electronic structure of g- C3N4/TiO2 induced by the presence of the metal single atoms are beneficial also for photocatalytic applications.
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  • 文章类型: Journal Article
    重构是催化反应中的重要现象。具有合适的氧化还原电势的转化型材料可以进行原位电化学驱动的重组并在工作的锂-硫电池中诱导高活性催化位点。在这里,在BiVO4电化学转化反应的驱动下,构建了Bi/非晶Li3VO4(a-Li3VO4)和Bi2S3/a-Li3VO4异质结的可逆催化循环,目标是Li2S的氧化和多硫化物的转化,分别。异质结构和电化学驱动的尺寸限制为穿梭限制和硫转化提供了丰富的场所。尤其是,p-blockBi和Bi2S3可以通过p-p轨道杂化大大降低Li2S和多硫化物的转换能垒,促进硫阴极的双向反应。因此,在10.3mgcm-2的高硫负载和0.38mAcm-2的电流密度下,经过120次循环,相应的硫阴极具有7.5mAhcm-2的高可逆容量。本研究提供了一种可行的方案,通过利用电化学诱导的重组获得用于双向硫氧化还原的高效催化剂。
    Restructuring is an important phenomenon in catalytic reactions. Conversion-type materials with suitable redox potential may undergo in situ electrochemically driven restructurings and induce highly active catalytic sites in a working lithium-sulfur battery. Herein, driven by the electrochemical conversion reaction of BiVO4, a reversible catalytic cycle of Bi/amorphous Li3VO4 (a-Li3VO4) and Bi2S3/a-Li3VO4 heterojunctions is constructed, which targets the oxidation of Li2S and the conversion of polysulfide, respectively. The heterostructures and electrochemically driven size confinement provide abundant sites for shuttle restraining and sulfur conversion. Especially, the p-block Bi and Bi2S3 could dramatically reduce the conversion energy barriers of Li2S and polysulfide by virtue of the p-p orbital hybridization, promoting bidirectional reactions of the sulfur cathode. As a result, the corresponding sulfur cathode possesses a high reversible capacity of 7.5 mAh cm-2 after 120 cycles under a high sulfur loading of 10.3 mg cm-2 with a current density of 0.38 mA cm-2. This study furnishes a feasible scheme to obtain highly effective catalysts for bidirectional sulfur redox by utilizing the electrochemically induced restructuring.
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