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Atomic-ScaleMapping of an Emergent Interfacial Two-DimensionalElectron Gas at Anatase/LaAlO3 锐钛矿/LaAlO3界面二维电子气体的原子尺度映射
IF 10.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-10-14 DOI: 10.1021/acs.nanolett.6c01308
Michael Oberaigner,Manuel Ederer,Sandeep K. Chaluvadi,Pasquale Orgiani,Regina Ciancio,Stefan Löffler,Gerald Kothleitner,Daniel Knez
Abstract Atomic-level insight into structure, charge distribution, chemistry, and electronic states is essential for understanding emergent properties at oxide interfaces. Here, we leverage the quasi-strain-free anatase TiO2/LaAlO3 interface as an ideal model system to decouple intrinsic polar discontinuities from complex strain artifacts. By combining atomic-resolution electron energy loss spectroscopy with integrated differential phase contrast, we spatially map the electronic states associated with the formation of a two-dimensional electron gas (2DEG). This correlative approach enables the direct real-space disentanglement of intrinsic 2DEG-related states from extrinsic Ti3+ defect states. Supported by density functional theory and inelastic scattering simulations, we reveal a physical superposition: the intrinsic polar electronic reconstruction anchors metallic states directly at the boundary, while oxygen vacancies accumulate further into the film, acting as a donor reservoir. This work not only resolves long-standing ambiguities regarding oxide interfacial conductivity but also provides a robust, transferable framework for related material systems.
原子水平上对结构、电荷分布、化学和电子态的洞察对于理解氧化物界面上的涌现特性是必不可少的。在这里,我们利用准无应变锐钛矿TiO2/LaAlO3界面作为理想的模型系统,从复杂的应变伪像中解耦本征极性不连续。通过结合原子分辨率电子能量损失光谱和积分微分相衬,我们在空间上绘制了与二维电子气(2DEG)形成相关的电子态。这种相关的方法使得从外在Ti3+缺陷态中直接解纠缠本征2deg相关态成为可能。在密度泛函理论和非弹性散射模拟的支持下,我们揭示了一种物理叠加:本然极性电子重构将金属态直接锚定在边界上,而氧空位则进一步积累到薄膜中,充当供体储层。这项工作不仅解决了长期以来关于氧化物界面电导率的模糊问题,而且为相关材料系统提供了一个强大的、可转移的框架。
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引用次数: 0
Erbium Probes of Magnetic Order in a van der Waals Material 范德华材料中磁序铒探针
IF 10.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-10-13 DOI: 10.1021/acs.nanolett.6c03698
Guadalupe García-Arellano,Gabriel I. López-Morales,Kang Xu,Samra Husremović,Jiayi Li,Arun Ramanathan,Xavier Roy,Cyrus E. Dreyer,Carlos A. Meriles
Embedded atomic emitters offer a complementary approach to characterizing magnetism in two-dimensional materials by accessing the magnetic environment from within. Here, we demonstrate that ion-implanted Er3+ centers act as internal optical probes in the van der Waals antiferromagnet CrSBr. Temperature-dependent telecom photoluminescence reveals signatures of the magnetic transition, persistent local magnetic behavior above the bulk Néel temperature, pronounced thermal hysteresis, and redistribution of optical spectral weight near the transition. Upon cooling, the Er resonances sharpen to the instrumental limit, pointing to remarkably homogeneous local environments despite implantation. Measurements spanning a 20-fold range of implantation fluence, structural characterization, and first-principles calculations suggest that the detected emission originates predominantly from an optically active subset of Er centers occupying well-defined environments and minimally perturbing the host magnetism. These results establish rare-earth defects as embedded probes of local magnetism and open opportunities for quantum-optical interrogation at individual lattice sites.
嵌入式原子发射器提供了一种互补的方法,通过从内部访问磁性环境来表征二维材料中的磁性。在这里,我们证明了离子注入Er3+中心在范德华反铁磁体CrSBr中充当内部光学探针。温度依赖的电信光致发光揭示了磁转变的特征,持续的局部磁行为高于体nsamel温度,明显的热滞后,以及在转变附近的光谱重分布。冷却后,Er共振锐化到仪器极限,尽管植入,但指向非常均匀的局部环境。测量跨越20倍的注入通量范围,结构表征和第一性原理计算表明,探测到的发射主要来自一个光学活跃的Er中心子集,占据明确定义的环境,并且对宿主磁性的干扰最小。这些结果确立了稀土缺陷作为局部磁性的嵌入探针,并为在单个晶格点上进行量子光学探测提供了机会。
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引用次数: 0
Dielectric Interfaces Reshape Dynamic Single-Molecule Optical Fingerprints in Nanometer-Thick Polymer Films 介质界面重塑纳米厚聚合物薄膜中的动态单分子光学指纹
IF 10.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-10-13 DOI: 10.1021/acs.nanolett.6c04137
Daniel Marx,David Malsbenden,Ivan Gligonov,Dominik Wöll,Jörg Enderlein,Oleksii Nevskyi
Fluorescence lifetimes near dielectric interfaces depend on molecular dipole orientation, but this relationship becomes more complex when emitters are confined within finite nanometer-thick polymer films. Here, we combine radially polarized excitation imaging with time-correlated single-photon counting to follow the orientation and fluorescence lifetime of individual PDI molecules undergoing rotational motion in thin poly(n-butyl methacrylate) films. Orientation-sensitive fluorescence patterns were analyzed using vectorial wave-optical simulations, enabling dipole orientation and excited-state lifetime to be correlated over time for the same emitter. The lifetime–orientation relationships vary systematically with film thickness and between molecules within the same film. Electrodynamic calculations for the glass–polymer–air geometry reproduce the principal trends and show that the observed heterogeneity is consistent with different axial emitter positions. These results establish single molecular dipoles as probes of finite nanometer-thick dielectric environments.
介电界面附近的荧光寿命取决于分子偶极子取向,但当发射器被限制在有限纳米厚的聚合物薄膜中时,这种关系变得更加复杂。在这里,我们将径向偏振激发成像与时间相关的单光子计数结合起来,跟踪在薄聚甲基丙烯酸正丁酯薄膜中进行旋转运动的单个PDI分子的取向和荧光寿命。利用矢量波光学模拟分析了取向敏感的荧光模式,使偶极子取向和激发态寿命随着时间的推移与同一发射器相关。寿命-取向关系随膜厚和同一膜内分子间的变化而有系统的变化。玻璃聚合物-空气几何结构的电动力学计算再现了主要趋势,并表明观察到的非均质性与不同轴向发射器位置一致。这些结果建立了单分子偶极子作为有限纳米厚介电环境的探针。
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引用次数: 0
Photobattery Architectures to Suppress Charge Recombination 抑制电荷复合的光电电池结构
IF 10.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-10-13 DOI: 10.1021/acs.nanolett.6c02373
Kohei Shimokawa,Byung-Man Kim,Arvind Pujari,Hooman Abbasi,Tetsu Ichitsubo,Michael De Volder
Integrating solar energy conversion and storage into single-unit photobatteries offers compact energy supplies. However, achieving sufficient photovoltage to charge batteries without external bias remains a critical bottleneck for these devices. Here, we demonstrate that the photovoltage in Zn-ion photobatteries can be modulated and enhanced by selecting and structuring the photoactive materials strategically. Randomly dispersed electrode configurations are easy to manufacture but they can suffer from charge recombination. In our experiments, these yielded a negligible photovoltage of ∼0.01 V. In comparison, our proposed layer-by-layer design, integrating a solid-state dye-sensitized solar cell (DSSC) with an optimized spinel Zn–Mn oxide cathode, increased the photovoltage output to ∼1 V under 1-sun illumination. This dramatic performance enhancement is achieved by better control over interfaces and charge transport and establishes a strategy for improving the architecture of future photobatteries.
将太阳能转换和存储集成到单个光电池中可以提供紧凑的能源供应。然而,获得足够的光电压来为电池充电而没有外部偏置仍然是这些设备的关键瓶颈。在这里,我们证明了锌离子光电池中的光电压可以通过有策略地选择和构造光活性材料来调制和增强。随机分散的电极结构易于制造,但它们容易受到电荷复合的影响。在我们的实验中,这些产生了可忽略不计的光电压,约0.01 V。相比之下,我们提出的分层设计将固态染料敏化太阳能电池(DSSC)与优化的尖晶石Zn-Mn氧化物阴极集成在一起,在1个太阳照射下将光电压输出提高到1 V。这种戏剧性的性能增强是通过更好地控制界面和电荷传输来实现的,并为改进未来光电电池的结构建立了策略。
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引用次数: 0
A Skin-likeHydrogel with Multidimensional Fillersfor Stable Human–Machine Interaction 具有多维填料的类皮肤水凝胶用于稳定的人机交互
IF 10.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-10-13 DOI: 10.1021/acs.nanolett.6c03665
Shengxin Xiang,Lei Liu,Xiao Wei,Feixiang Gao,Yu Lin,Zhiwei Zhao,Xinkai Xie,Jun Wu
Abstract The deep integration of human–machine interface (HMI) technology and the Internet of Things (IoT) has imposed stringent new requirements for electronic skin (e-skin) in terms of flexibility, comfort, and high sensitivity. Herein we present a multiconductive network hydrogel e-skin (MCNHE-skin) based on a poly(vinyl alcohol) (PVA)/polyvinylpyrrolidone (PVP) dual-network matrix with polydopamine (PDA), carbon nanotubes (CNTs), and MXene as conductive fillers. The MCNHE-skin exhibits electrical conductivity (<5 kΩ), high stretchability (∼650%), strong self-adhesion (∼19 kPa), and low modulus (∼3.6 kPa). These characteristics enable its successful application in multimodal sensing systems such as strain sensors, pressure sensors, triboelectric nanogenerators (TENGs), and physiological signal monitors. Furthermore, by integration with flexible printed circuit boards (FPCBs), MCNHE-skin is developed into smart wearable systems for noncontact HMI. The 0D/1D/2D synergistic conductive network presented in this hydrogel e-skin yields high-fidelity sensing and noncontact control capabilities, marking a significant step forward in the development of multifunctional wearable electronics.
人机界面(HMI)技术与物联网(IoT)的深度融合,对电子皮肤(e-skin)在灵活性、舒适性、高灵敏度等方面提出了严格的新要求。在此,我们提出了一种基于聚乙烯醇(PVA)/聚乙烯吡咯烷酮(PVP)双网络基质的多导电网络水凝胶电子皮肤(MCNHE-skin),以聚多巴胺(PDA)、碳纳米管(CNTs)和MXene为导电填料。MCNHE-skin具有导电性(<5 kΩ)、高拉伸性(~ 650%)、强自粘附性(~ 19 kPa)和低模量(~ 3.6 kPa)。这些特性使其成功应用于多模态传感系统,如应变传感器、压力传感器、摩擦纳米发电机(TENGs)和生理信号监测器。此外,通过与柔性印刷电路板(fpcb)集成,MCNHE-skin发展成为非接触式人机界面的智能可穿戴系统。在这种水凝胶电子皮肤中提出的0D/1D/2D协同导电网络产生了高保真的传感和非接触控制能力,标志着多功能可穿戴电子产品的发展向前迈出了重要一步。
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引用次数: 0
Directional Manufacturing of Defect Mitigation and Large-Scale Single-Crystalline Metal Foils via Gas Flow Optimization toward Commercialization 定向制造的缺陷缓解和大规模单晶金属箔的气体流动优化走向商业化
IF 10.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-10-13 DOI: 10.1021/acs.nanolett.6c03824
The-Hung Mai,Thi H. Ho,Shi-Hui Liu,Santhoshkumar S,Muhammad Adnan,Arvind Chandrasekar,Tuan V. Vu,Chien-Cheng Kuo,Hung-Duen Yang,Liuwen Chang,Wei-Lung Tseng,Trung Nguyen-Thoi,Chung-Li Dong,Phuong V. Pham
Single-crystalline metals, with their distinctive symmetries, are the ideal medium for high-order molecular arrangement and the diminishing of grain boundaries and defect sites coupled with high anisotropy. However, conventional synthesis via bulk growth or epitaxial deposition remains complex, costly, and difficult to scale. Here, we report a simple and inexpensive strategy as an alternative to conventional strategies for manufacturing single-crystalline metal foils. Miraculously, by miniaturization of grain boundaries and promoting surface energy minimization during the rotation of the crystal lattice followed by the consumption of neighboring grains, high-quality and large-scale single-crystalline metal foils (Cu(111), Ni(111)) were obtained via vertically suspended chemical vapor deposition (CVD) annealing of polycrystalline metal foils. This discovery offers a potential strategy for manipulating and producing large-scale metal foils that may be used for industrial-scale applications.
单晶金属具有独特的对称性,是高阶分子排列、晶界和缺陷位置减小以及高各向异性的理想介质。然而,通过体生长或外延沉积的传统合成仍然复杂,昂贵且难以规模化。在这里,我们报告了一种简单而廉价的策略,作为制造单晶金属箔的传统策略的替代方案。通过对多晶金属箔进行垂直悬浮化学气相沉积(CVD)退火,通过晶格旋转过程中晶界的小型化和促进表面能的最小化,进而消耗邻近晶粒,获得了高质量和大规模的单晶金属箔(Cu(111), Ni(111))。这一发现为操纵和生产大规模金属箔提供了一种潜在的策略,可以用于工业规模的应用。
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引用次数: 0
Excitation-Wavelength-Dependent Dual Emission in Au42 Quantum Rods Au42量子棒中激发-波长相关的双发射
IF 10.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-10-12 DOI: 10.1021/acs.nanolett.6c04058
Guiying He,Lianshun Luo,Mircea Cotlet,Guoxiang Hu,Gangli Wang,Rongchao Jin
Dual emissive materials are of particular importance in chemical and biological assays. Herein, we focus on a rod-shaped Au42(SCH2CH2Ph)32 nanocluster that exhibits dual emission at 875 and 1040 nm owing to fluorescence (FL) and phosphorescence (PH), respectively. Transient absorption analysis shows a slow intersystem crossing (ISC, ∼500 ps) from lowest singlet S1 to triplet T1 upon direct S1 excitation, leading to dual emission from both S1 and T1. However, upon excitation of the higher Sn state, we observe a metastable singlet state (S′). We rationalize two competing decay pathways from S′: (i) internal conversion to S1 and (ii) ISC to high triplet Tn≥2. These processes alter the populations of the S1 and T1 states, which explains the excitation-wavelength-dependent dual emission and FL/PH ratios. The revealed excited-state mechanism and the dual emissive Au42 material will serve as a paradigm for future research on atomically precise nanoclusters.
双发射材料在化学和生物分析中特别重要。本文研究了一种杆状的Au42(SCH2CH2Ph)32纳米簇,该簇在875 nm和1040 nm处分别由于荧光(FL)和磷光(PH)表现出双重发射。瞬态吸收分析表明,在S1直接激发下,从最低单重态S1到三重态T1有一个缓慢的系统间交叉(ISC, ~ 500 ps),导致S1和T1双重发射。然而,当激发高Sn态时,我们观察到一个亚稳态单重态(S ')。我们从S '合理化了两种竞争的衰变途径:(i)内部转换到S1和(ii) ISC到高三重态Tn≥2。这些过程改变了S1和T1态的居群,这解释了激发波长相关的双发射和FL/PH比。揭示的激发态机制和双发射Au42材料将为未来原子精密纳米团簇的研究提供一个范例。
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引用次数: 0
From Micro to Nano: Boosting γ-MnO2 Cathode Performance through Particle Size Engineering 从微观到纳米:通过粒度工程提高γ-MnO2阴极性能
IF 10.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-10-12 DOI: 10.1021/acs.nanolett.6c04092
Ella Davidi,Isaac Loke,Samuel Eisenberg,Xinzhe Xue,Megan C. Freyman,Asya Orhan,Erika P. Ramos,Jianchao Ye,Seongkoo Cho,Makena White,Christopher Nelson,Hanyu Wang,Christine A. Orme,Bruce Dunn,Marcus A. Worsley,Yat Li
Fast-charging lithium-ion batteries require cathodes that sustain rapid Li+ transport while maintaining structural and interfacial stability. Here, we investigate particle-size effects in γ-MnO2 by comparing micron-sized (4.4 ± 0.8 μm) and nanosized (62 ± 21 nm) particles under identical conditions. Nanosized γ-MnO2 delivers 160.1 mAh g–1 at C/10 and retains ∼66% capacity at 5C while exhibiting lower charge-transfer and diffusion-related impedance. Cyclic voltammetry and Dunn’s analysis reveal a 68.9% capacitive contribution at 2 mV s–1, indicating a shift toward faster surface-controlled charge storage enabled by increased surface area and shorter Li+ diffusion pathways. GITT measurements show deeper lithiation (x ≈ 0.65 vs 0.48 in LixMnO2) and a more homogeneous solid-solution-like intercalation regime in nanosized particles, avoiding bulk phase-transition kinetic bottlenecks. The nanosized cathode retains 70% capacity with ∼99.5% Coulombic efficiency after 400 cycles at 3C, demonstrating particle-size engineering as an effective strategy for high-rate, long-life advanced battery energy storage.
快速充电的锂离子电池要求阴极在保持结构和界面稳定性的同时保持Li+的快速传输。本文通过比较微米(4.4±0.8 μm)和纳米(62±21 nm)颗粒在相同条件下对γ-MnO2的粒径影响进行了研究。纳米尺寸的γ-MnO2在C/10时提供160.1 mAh g-1,在5C时保持约66%的容量,同时表现出较低的电荷转移和扩散相关阻抗。循环伏安法和Dunn的分析显示,在2mv s-1下,电容性贡献为68.9%,表明通过增加表面积和缩短Li+扩散路径,可以实现更快的表面控制电荷存储。GITT测量结果显示,LixMnO2的锂化程度更深(x≈0.65 vs 0.48),并且在纳米颗粒中具有更均匀的类似固溶体的插层结构,避免了大块相变动力学瓶颈。该纳米级阴极在3C下循环400次后仍能保持70%的容量和99.5%的库仑效率,证明了粒径工程是高速率、长寿命先进电池储能的有效策略。
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引用次数: 0
Polyaniline-Modified MXene/Carbon Nanotube Scaffold Enabling High-Rate and Long-Cycle Zinc–Iodine Batteries 聚苯胺修饰MXene/碳纳米管支架制备高倍率长循环锌碘电池
IF 10.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-10-12 DOI: 10.1021/acs.nanolett.6c04159
Xiaoqian Gong,Yixing Wang,Mengya Ge,Qinghong Wang
Aqueous zinc–iodine (Zn–I2) batteries are attractive for large-scale energy storage because of their low cost and inherent safety. However, the practical use of an I2 cathode is severely restricted by poor electronic conductivity and the shuttle effect of soluble polyiodides. Herein, a synergistic scaffold composed of MXene and carbon nanotubes (CNTs) modified with protonated polyaniline (PANI) via electrostatic interactions was designed. The MXene/CNT scaffold ensures overall conductivity and structural integrity. The protonated PANI immobilizes iodine species through nitrogen-containing groups and accelerates their interconversion, effectively suppressing the shuttle effect. The MXene/CNTs/PANI-I2 cathode with an iodine loading of 43.96 wt % achieves a superior specific capacity of 150 mAh g–1 at a high rate of 20 C as well as excellent cycling stability over 10 000 cycles. This work offers a viable strategy for developing stable I2 cathodes for high-performance Zn–I2 batteries.
水相锌碘(Zn-I2)电池由于其低成本和固有的安全性,在大规模储能方面具有很大的吸引力。然而,I2阴极的实际使用受到电子导电性差和可溶性多碘化物的穿梭效应的严重限制。本文设计了一种由MXene和经质子化聚苯胺(PANI)修饰的碳纳米管(CNTs)通过静电相互作用组成的协同支架。MXene/CNT支架可确保整体导电性和结构完整性。质子化聚苯胺通过含氮基团固定碘,加速其相互转化,有效抑制穿梭效应。碘负载为43.96 wt %的MXene/CNTs/PANI-I2阴极在20℃的高倍率下具有150 mAh g-1的优越比容量以及超过10 000次循环的优异循环稳定性。这项工作为开发高性能锌- I2电池的稳定I2阴极提供了一种可行的策略。
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引用次数: 0
Interface-Induced Crystallographic Orientation of Zinc Deposition Enabled by a Zwitterionic Dynamic Buffering Interface for Ultralong-Life Aqueous Zinc Batteries 超长寿命锌水电池中两性离子动态缓冲界面诱导锌沉积的晶体取向
IF 10.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-10-12 DOI: 10.1021/acs.nanolett.6c03526
Xin Wei,Qing-Yuan Zhao,Ji-Zun Zhang,Hai Xu,Zi-Yan Liu,Naoyuki Shibayama,Yu-Ting Xu,Xiao-Feng Wang
The development of aqueous zinc batteries is critically constrained by the electrode–electrolyte interfacial instability at the Zn anode. Herein, a zwitterionic dynamic buffering interface (ZDBI) is constructed by using trace glufosinate ammonium (GA). The dissociated GA– anchors onto the Zn(101) surface via its phosphinate and carboxylate groups with its protonated amino group (−NH3+) extending into the electrolyte to dynamically respond to interfacial electric fields. Meanwhile, free NH4+ cations can form an electrostatic shielding layer under an electric field. This synergistic chemisorbed-mobile-ion buffering network thickens the electric double layer, inhibits water-splitting parasitic reactions, and induces (101)-oriented deposition. Consequently, Zn||Zn symmetric cells sustain stable cycling for over 7800 h with a cumulative capacity of 3.9 Ah cm–2, while Zn||Cu half-cells achieve an average Coulombic efficiency of 99.3%, and Zn||V2O5 full cells retain 88% capacity after 1000 cycles at 5 A g–1. This work offers an efficient strategy for addressing electrode–electrolyte interfacial issues.
锌阳极电极-电解质界面的不稳定性严重制约了锌水溶液电池的发展。本文采用微量草铵(GA)构建了两性离子动态缓冲界面(ZDBI)。解离的GA -通过其磷酸基和羧酸基锚定在Zn(101)表面,其质子化氨基(- NH3+)延伸到电解质中,动态响应界面电场。同时,游离NH4+阳离子在电场作用下形成静电屏蔽层。这种协同的化学吸收-移动离子缓冲网络增厚了双电层,抑制了水分解寄生反应,并诱导了(101)定向沉积。因此,Zn||Zn对称电池可稳定循环超过7800 h,累积容量为3.9 Ah cm-2,而Zn||Cu半电池可实现99.3%的平均库仑效率,Zn||V2O5全电池在5 a g-1下循环1000次后仍保持88%的容量。这项工作为解决电极-电解质界面问题提供了一种有效的策略。
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引用次数: 0
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