Nano Letters最新文献

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How Cation Rigidity and Dipole Moment Prolong Hot-Carrier Lifetime in 2D Perovskites. 阳离子刚度和偶极矩如何延长二维钙钛矿的热载子寿命。

IF 10.8 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters

Pub Date : 2026-01-31 DOI: 10.1021/acs.nanolett.5c05918

Zeping Ou,Yu Jie Zheng,Wei Fang,Yi Pan,Liyuan Jiang,Kuan Sun

2D Dion-Jacobson perovskites are promising solar cells due to high efficiency and stability yet are limited by poor charge dynamics and energy loss. Using density functional theory, ab initio molecular dynamics, and nonadiabatic molecular dynamics simulations to explore the cation rigidity and dipole moment of cations can extend hot-carrier lifetime and slow down charge recombination. Specifically, increasing the cation dipole moment strengthens hydrogen bonding between the organic spacer and the inorganic lattice, while a rigid cation enhances lattice stiffness. These factors strengthen thermal coupling between the organic and [PbI6]4- inorganic framework, reduce atomic fluctuations, and induce phonon softening. This suppresses nonadiabatic coupling and shifts dominant electron-phonon interactions of high-frequency modes to low-frequency modes, thereby prolonging hot-carrier lifetime and reducing nonradiative recombination. Thus, dipole engineering primarily enhances hot-carrier lifetime by suppressing nonradiative pathways, rather than accelerating hot-carrier cooling. Our finding provides guidelines for designing more efficient and stable perovskite solar cells.

二维Dion-Jacobson钙钛矿是一种很有前途的太阳能电池，由于其高效率和稳定性，但受到电荷动力学和能量损失的限制。利用密度泛函理论、从头算分子动力学和非绝热分子动力学模拟来探讨阳离子的刚性和偶极矩对延长热载子寿命和减缓电荷复合的作用。具体来说，增加阳离子偶极矩加强了有机间隔剂和无机晶格之间的氢键，而刚性阳离子增强了晶格刚度。这些因素增强了有机骨架和[PbI6]4-无机骨架之间的热耦合，减少了原子波动，并诱导声子软化。这抑制了非绝热耦合并将高频模式的主导电子-声子相互作用转移到低频模式，从而延长了热载子寿命并减少了非辐射复合。因此，偶极子工程主要通过抑制非辐射途径来提高热载子寿命，而不是加速热载子冷却。我们的发现为设计更高效、更稳定的钙钛矿太阳能电池提供了指导。

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引用次数: 0

Two-Dimensional Metal-Organic Framework for Supercapacitors: Thickness-Dependent Charge Storage Mechanisms. 超级电容器的二维金属-有机框架：厚度相关电荷存储机制。

IF 10.8 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters

Pub Date : 2026-01-31 DOI: 10.1021/acs.nanolett.5c06178

Hiran Jyothilal,Sabiar Rahaman,Vikas Sharma,Kavita Pandey,Ashok Keerthi,Boya Radha

Additive-free active materials are desirable for energy storage devices as they reduce processing complexity and eliminate variability from binders or conductive additives. We report the synthesis of a highly stable, two-dimensional copper-based metal-organic framework (CuMOF) film with a tunable thickness. The exceptional adhesion of CuMOF films to electrode surfaces enables a binder-free fabrication approach, addressing a key challenge in energy storage applications, particularly in electrode design. The film exhibits a columnar morphology with well-defined grain boundaries and a high surface area, making it optimal for supercapacitor applications. Electrochemical characterization on glassy carbon electrodes yielded an areal capacitance of 2.9 mF/cm2 at a scan rate of 1 mV/s using a ∼160 nm thick CuMOF film. We investigated films as thin as 2.4 nm, where the capacitance is predominantly governed by electrical double-layer effects, highlighting the interplay between the film structure and electrochemical behavior. Thus, CuMOF films offer practical applicability, advancing efficient binder-free energy storage.

无添加剂的活性材料是能量存储设备的理想选择，因为它们降低了加工的复杂性，消除了粘合剂或导电添加剂的可变性。我们报道了一种高度稳定的，具有可调厚度的二维铜基金属有机框架（CuMOF）薄膜的合成。CuMOF薄膜与电极表面的特殊附着力使无粘结剂的制造方法成为可能，解决了储能应用中的关键挑战，特别是在电极设计方面。该薄膜呈现柱状形态，具有明确的晶界和高表面积，使其成为超级电容器应用的最佳选择。利用~ 160 nm厚的CuMOF薄膜，在1 mV/s的扫描速率下，对玻碳电极进行电化学表征，得到2.9 mF/cm2的面电容。我们研究了厚度为2.4 nm的薄膜，其中电容主要由电双层效应控制，突出了薄膜结构和电化学行为之间的相互作用。因此，CuMOF薄膜具有实际的适用性，推进了高效的无粘结剂储能。

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引用次数: 0

Concurrent Enhancement of Thermopower and Conductivity via Modulation of Diacetylide-Electrode Coupling in Molecular Junctions 通过分子结中二乙酰基-电极耦合的调制来同时增强热功率和电导率

IF 10.8 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters

Pub Date : 2026-01-31 DOI: 10.1021/acs.nanolett.5c05618

Jiung Jang, Yuya Tanaka, Danbi Lee, Peng He, Tatsuhiko Ohto, Zee Hwan Kim, Hyo Jae Yoon

The study of molecular thermoelectricity offers fundamental insights into charge transport via tunneling through organic and organometallic systems, with implications for nanoscale energy conversion technologies. Here, we investigate how molecule–electrode coupling strength influences thermoelectric performance in molecular junctions incorporating self-assembled monolayers of π-extended Ru(dppe)₂-diacetylide complex. Surface modification of gold electrode with monatomic Pt and Pd layers via underpotential deposition enabled precise tuning of the strength of molecule–electrode contact. This tuning enhanced electronic interaction with the remotely positioned Ru core, promoted cumulene-like π-delocalization along the molecular backbone, reorganized frontier orbitals, and simultaneously enhanced the Seebeck coefficient and electrical conductivity to amplify the power factor by up to 111-fold compared to unmodified junctions. These findings highlight the broader potential of diacetylide complex to translate subtle orbital interactions into significant energy-conversion functions.

分子热电的研究为通过有机和有机金属系统的隧道传输电荷提供了基本的见解，对纳米级能量转换技术具有重要意义。本文研究了分子-电极耦合强度对π-延伸钌（dppe）2-二乙酰基配合物自组装单层分子结热电性能的影响。利用欠电位沉积方法对单原子铂和钯层金电极进行表面修饰，实现了分子电极接触强度的精确调谐。这种调谐增强了与远程定位的Ru核的电子相互作用，促进了沿分子骨干的类累积π离域，重组了前沿轨道，同时提高了塞贝克系数和电导率，使功率因数比未修饰的结放大了111倍。这些发现强调了二乙酰基配合物将微妙的轨道相互作用转化为重要的能量转换功能的更广泛的潜力。

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引用次数: 0

Interfacial Bond Dipole Engineering for Accelerated Photogenerated Charge Migration in a Red Phosphorus Based Heterojunction. 红磷基异质结中加速光生电荷迁移的界面键偶极子工程。

IF 10.8 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters

Pub Date : 2026-01-30 DOI: 10.1021/acs.nanolett.5c05969

Yingnan Duan,Hexiang Zhao,Tianhao Li,Jixiang Ji,Yuanxing Fang,Jimmy C Yu,Zhurui Shen,Xinchen Wang

Gaining in-depth insights into the interfacial dipole is crucial for optimizing the transfer kinetics of photogenerated electrons at heterojunction interfaces. Herein, we establish interfacial bond polarity as a universal descriptor governing electron transfer kinetics, demonstrated via two model heterojunctions (RP/S8 and RP/CdS) with identical P-O-S bonds. Density functional theory (DFT) calculation revealed a stronger interfacial dipole in RP/CdS (2.75 D) than in RP/S8 (1.83 D). Femtosecond transient absorption spectroscopy (fs-TAS) demonstrates a pronounced acceleration of interfacial electron transfer, with RP/CdS exhibiting a rate constant of 5.5 × 109 s-1, significantly exceeding that of RP/S8 (2.5 × 108 s-1). The stronger interface dipole is the key to facilitating the efficient migration of charges. Consistently, the photocatalytic hydrogen evolution (PHE) activities of RP/S8 and RP/CdS were 1.5-fold and 4.5-fold enhanced compared with their corresponding mechanical mixtures, respectively. This study highlights interfacial dipole engineering as a powerful strategy for the rational design of high-efficiency heterojunction photocatalysts.

深入了解界面偶极子对于优化异质结界面光生电子的转移动力学至关重要。本文通过两种具有相同P-O-S键的异质结（RP/S8和RP/CdS）模型，建立了界面键极性作为控制电子转移动力学的通用描述符。密度泛函理论（DFT）计算表明，RP/CdS （2.75 D）比RP/S8 （1.83 D）具有更强的界面偶极子。飞秒瞬态吸收光谱（fs-TAS）表明，RP/CdS的界面电子转移速率常数为5.5 × 109 s-1，明显超过RP/S8 （2.5 × 108 s-1）。较强的界面偶极子是促进电荷有效迁移的关键。RP/S8和RP/CdS的光催化析氢活性分别比其相应的机械混合物提高1.5倍和4.5倍。本研究强调界面偶极子工程是合理设计高效异质结光催化剂的有力策略。

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引用次数: 0

Electron Beam Manipulation on the Moiré Superlattice of Bilayer WS2 电子束对双层WS2莫尔维尔超晶格的操纵

IF 10.8 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters

Pub Date : 2026-01-30 DOI: 10.1021/acs.nanolett.5c05946

Xiaohui Zeng, Chuang Tian, Dong Zhang, Guanghui Yu, Yuan Hu, Jun Li, Kecheng Cao

The moiré superlattice in twisted transition metal dichalcogenides (TMDCs) offers a versatile platform for exploring electronic properties and correlated quantum phenomena. However, conventional fabrication methods using transfer and stacking techniques suffer from interfacial contamination and limited scalability. Here, we introduce an in situ focused electron beam irradiation approach to dynamically manipulate and characterize the moiré superlattice in bilayer 2H-WS₂ in TEM. We achieve real-time moiré pattern control, enabling precise twist angle adjustments (6–10°). Prolonged irradiation induces displacement of tungsten (W) and sulfur (S) atoms from the moiré superlattice, which migrate to heal vacancies in adjacent monolayers, ultimately collapsing the superlattice into a WS₂ monolayer and revealing an unexpected atomic-scale self-repair mechanism. This technique advances the study of twistronics in 2D quantum materials by providing a pathway for atomically precise engineering of moiré-driven electronic states while highlighting the potential of electron beam lithography (EBL) for the controllable fabrication of moiré devices.

扭曲过渡金属二硫族化合物（TMDCs）中的莫尔维尔超晶格为探索电子性质和相关量子现象提供了一个通用的平台。然而，使用转移和堆叠技术的传统制造方法存在界面污染和可扩展性有限的问题。在这里，我们引入了一种原位聚焦电子束辐照的方法来动态操纵和表征双层2H-WS2的摩尔超晶格。我们实现实时波纹模式控制，实现精确的扭转角度调整（6-10°）。长时间的辐照导致钨(W)和硫(S)原子从莫尔维尔超晶格中位移，这些原子迁移到邻近单层的空位上，最终将超晶格坍塌成WS2单层，并揭示了意想不到的原子尺度的自修复机制。该技术通过提供一种原子精确工程的途径来实现莫伊莫尔驱动的电子态，同时突出了电子束光刻（EBL）在莫伊莫尔器件的可控制造方面的潜力，从而推进了二维量子材料中扭曲电子学的研究。

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引用次数: 0

Water Clusters Act as a Nano-Steam Engine in Covalent Organic Framework Nanochannels for Boosting Solid-State Li-Ion Conduction and Electrochemical Stability. 在共价有机框架纳米通道中，水团簇作为纳米蒸汽机提高固态锂离子的导电性和电化学稳定性。

IF 10.8 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters

Pub Date : 2026-01-30 DOI: 10.1021/acs.nanolett.5c05523

Juan Li,Dongsheng Wang,Linrong Yue,Yukun Liu,Xuan Tang

The development of solid-state electrolytes (SSE) that combine high ionic conductivity with a wide electrochemical window remains a significant challenge. This work presents a novel "nano-steam engine" concept within the one-dimensional nanochannels of urea-linked covalent organic frameworks (COFs) to address this challenge. By leveraging the strong anchoring effect of urea groups on water clusters, a fast lithium-ion conductor was developed by using the hydrophilicity of lithium salts. This design strategy promotes the dissociation of lithium salts and establishes a low-energy pathway for ion migration, achieving exceptional room-temperature ionic conductivity of 1.5 × 10-3 S cm-1. Meanwhile, the strong anchoring effect of the urea group on water clusters effectively suppressed the hydrogen evolution reaction, enabling the electrochemical window of the hydrated SSE to exceed 4.8 V. The assembled solid-state LiMn2O4//Li4Ti5O12 battery demonstrated a stable charge/discharge over 100 cycles. This study provides a groundbreaking strategy for designing high-performance solid-state lithium-ion batteries by turning water into a promoter of lithium-ion conduction.

结合高离子电导率和宽电化学窗口的固态电解质（SSE）的发展仍然是一个重大挑战。本研究提出了一种新颖的“纳米蒸汽机”概念，该概念在脲联共价有机框架（COFs）的一维纳米通道内解决了这一挑战。利用脲基对水团簇的强锚定效应，利用锂盐的亲水性开发了一种快速锂离子导体。这种设计策略促进了锂盐的解离，并建立了离子迁移的低能途径，实现了1.5 × 10-3 S cm-1的优异室温离子电导率。同时，尿素基团对水团簇的强锚定作用有效抑制了析氢反应，使水合SSE的电化学窗口超过4.8 V。所组装的固态LiMn2O4//Li4Ti5O12电池具有超过100次循环的稳定充放电性能。这项研究为设计高性能固态锂离子电池提供了突破性的策略，将水转化为锂离子传导的促进剂。

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引用次数: 0

In Situ Magnetism Decoupling Gradient-Regulated Mn-O Interaction Mechanism on Stabilizing Li-Rich Cathodes. 稳定富锂阴极的原位磁去耦梯度调节Mn-O相互作用机理。

IF 10.8 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters

Pub Date : 2026-01-30 DOI: 10.1021/acs.nanolett.5c05845

Shiyu Qiu,Jin Bai,Peiyao Wang,Ke Xiao,Yuanyuan Liu,Siya Wang,Xuebin Zhu,Yao Xiao,Bangchuan Zhao,Yuping Sun

Lithium-rich layered oxides are promising high-capacity cathodes for lithium-ion batteries, but their commercialization is hindered by severe capacity loss and voltage decay. Herein, we develop a full concentration gradient Li-rich Mn-based layered oxide with gradually decreased Mn and increased Ni concentration from the center to the surface. The gradient material delivers exceptional cycling stability and rate capability, offering a high capacity of 216 mAh g-1 at 1 C and outstanding retention of 91.8% after 200 cycles at 2 C. To elucidate the underlying atomic-level interaction mechanism behind them, in situ magnetism characterization is employed and reveals that the gradient design effectively stabilizes Mn-O interaction and suppresses O-O dimer formation, alleviating irreversible anionic oxygen redox and undesirable structural degradation after long-term cycling. This work affords an effective gradient strategy to regulate the Mn-O interaction, opening up a new perspective for developing Li-rich Mn-based cathode materials.

富含锂的层状氧化物是锂离子电池的高容量阴极，但其商业化受到严重容量损失和电压衰减的阻碍。在此，我们开发了一种完全浓度梯度的富锂锰基层状氧化物，从中心到表面Mn浓度逐渐降低，Ni浓度逐渐增加。该梯度材料具有优异的循环稳定性和速率能力，在1℃下提供216 mAh g-1的高容量，在2℃下200次循环后提供91.8%的优异保留率。为了阐明其背后的原子水平相互作用机制，采用原位磁性表征，揭示了梯度设计有效地稳定了Mn-O相互作用并抑制了O-O二聚体的形成。缓解不可逆的阴离子氧氧化还原和长期循环后不良的结构降解。这项工作提供了一种有效的梯度策略来调节Mn-O相互作用，为开发富锂mn基正极材料开辟了新的前景。

引用次数: 0

Emergent Synchronization and Self-Organization of Autonomous Nanospinners 自主纳米纺丝体的紧急同步与自组织

IF 10.8 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters

Pub Date : 2026-01-30 DOI: 10.1021/acs.nanolett.5c05293

Tahniat Afsari, Suzanne Ahmed

Autonomous, self-propelled, nanoscale particles, have sparked significant research interest due to their ability to serve as models for understanding the physical principles governing the individual and collective behaviors of living and nonliving systems at low Reynolds numbers. These systems also have many potential applications in drug delivery, environmental remediation, sensing, and oil recovery. However, most research has focused on particles undergoing linear motion, leaving a gap in the understanding of autonomous rotating systems. Addressing this gap would provide crucial insights into the nature of interactions and collective behaviors of rotating systems and enable applications such as nanomixing. In this work, we present the novel design and facile, high yield synthesis of autonomous nanospinners capable of achieving high frequency rotation. We report the evolution of their phase relationships, their emergent synchronization, and the self-organization of multiple spinners, marking a key step toward understanding the emergent behavior of autonomous nanoscale spinners.

自主的、自我推进的纳米级粒子，由于能够作为模型来理解在低雷诺数下控制生命和非生命系统的个体和集体行为的物理原理，已经引发了重大的研究兴趣。这些系统在药物输送、环境修复、传感和石油开采方面也有许多潜在的应用。然而，大多数研究都集中在进行线性运动的粒子上，这在对自主旋转系统的理解上留下了空白。解决这一差距将为了解旋转系统的相互作用和集体行为的本质提供重要的见解，并使纳米混合等应用成为可能。在这项工作中，我们提出了能够实现高频旋转的自主纳米纺丝的新颖设计和简便，高产率合成。我们报道了它们的相位关系的演变，它们的紧急同步，以及多个旋转器的自组织，这标志着理解自主纳米级旋转器的紧急行为的关键一步。

引用次数: 0

Mie-Void-Enabled WS₂ Excitonic Emitters with Nanoscale Footprints. 具有纳米尺寸足迹的mii - void - enabled WS2激子发射器。

IF 9.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters

Pub Date : 2026-01-30 DOI: 10.1021/acs.nanolett.5c05977

Yinchang Liao, Yuhua Chen, Yuefeng Wang, Meng Xia, Kai Ding, Tao Wang, Xingwang Zhang

Owing to their strong excitonic effects, monolayer transition metal dichalcogenides (1L TMDs) are highly promising for next-generation excitonic light-emitting devices. To enhance exciton emission, 1L TMDs are typically integrated with dielectric optical resonators, which, however, results in a large footprint and/or interface-induced exciton emission suppression. To overcome these fundamental issues, we herein present the experimental demonstration of nanoscale tungsten disulfide (WS₂) excitonic light-emitting devices enabled by Mie voids. Such a Mie void not only supports a localized Mie resonance in the nanoscale air hole to enhance exciton emission but also suspends 1L WS₂ in the air to eliminate the emission suppression from the contact interface. When we leverage the nanoscale field localization within Mie voids, a high-resolution light-emitting display is realized with a pixel size of ∼1.12 μm. Our work opens a door to nanoscale 2D semiconductor light sources with potential applications in a high-resolution light-emitting display.

由于具有较强的激子效应，单层过渡金属二硫族化合物（1L tmd）在下一代激子发光器件中具有很大的应用前景。为了增强激子发射，1L tmd通常与介电光学谐振器集成在一起，然而，这导致了大的占地面积和/或界面诱导的激子发射抑制。为了克服这些基本问题，我们在此提出了由Mie空洞实现的纳米级二硫化钨（WS2）激子发光器件的实验演示。这种Mie空洞不仅在纳米尺度的空穴中支持局域Mie共振以增强激子发射，而且在空气中悬浮1L WS2以消除接触界面的发射抑制。当我们利用Mie空隙内的纳米级场定位时，实现了像素尺寸为1.12 μm的高分辨率发光显示器。我们的工作为纳米级二维半导体光源在高分辨率发光显示器中的潜在应用打开了一扇门。

引用次数: 0

Sensing Single-Molecule Magnets with Nitrogen-Vacancy Centers. 氮空位中心感应单分子磁体。

IF 9.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters

Pub Date : 2026-01-29 DOI: 10.1021/acs.nanolett.5c05066

Ariel Smooha, Jitender Kumar, Dan Yudilevich, John W Rosenberg, Valentin Bayer, Rainer Stöhr, Andrej Denisenko, Tatyana Bendikov, Anna Kossoy, Iddo Pinkas, Hengxin Tan, Binghai Yan, Biprajit Sarkar, Joris van Slageren, Amit Finkler

Single-molecule magnets (SMMs) are molecules that can function as nanoscale magnets with potential use as magnetic memory bits. While SMMs can retain magnetization at low temperatures, characterizing them on surfaces and at room temperature remains challenging and requires specialized nanoscale techniques. Here, we use single nitrogen-vacancy (NV) centers in diamond as a highly sensitive, broadband magnetic field sensor to detect the magnetic noise of cobalt-based SMMs deposited on a diamond surface. We measured the NV relaxation and decoherence times at 296 K and at 5-8 K, observing a significant influence of the SMMs on them. From this, we infer the SMMs' magnetic noise spectral density (NSD) and underlying magnetic properties. Moreover, we observe the effect of an applied magnetic field on the SMMs' NSD at low temperatures. The method provides nanoscale sensitivity for characterizing SMMs under realistic conditions relevant to their use as surface-bound memory units.

单分子磁体（SMMs）是一种可以作为纳米级磁体的分子，具有磁性存储位的潜在用途。虽然smm可以在低温下保持磁化，但在表面和室温下表征它们仍然具有挑战性，需要专门的纳米级技术。在这里，我们使用金刚石中的单氮空位（NV）中心作为高灵敏度的宽带磁场传感器来检测沉积在金刚石表面的钴基smm的磁噪声。我们在296 K和5-8 K测量了NV弛豫和退相干时间，观察到smm对它们的显著影响。由此，我们推断出smm的磁噪声谱密度（NSD）和潜在的磁性能。此外，我们还观察了外加磁场对低温下smm的NSD的影响。该方法提供了纳米级的灵敏度，在实际条件下表征smm作为表面约束的存储单元。

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