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Deterministic Generation of Single B Centers in hBN by One-to-One Conversion from UV Centers UV中心一对一转换hBN中单B中心的确定性生成
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-25 DOI: 10.1021/acsnano.5c19102
Andrés Núñez Marcos, Christophe Arnold, Julien Barjon, Stéphanie Buil, Jean-Pierre Hermier, Aymeric Delteil
Among the variety of quantum emitters in hexagonal boron nitride (hBN), blue-emitting color centers, or B centers, have garnered particular interest owing to their excellent quantum optical properties. Moreover, the fact that they can be locally activated by an electron beam makes them suitable for top-down integration into photonic devices. However, in the absence of a real-time monitoring technique sensitive to individual emitters, the activation process is stochastic in the number of emitters, and its mechanism is under debate. Here, we implement an in situ cathodoluminescence monitoring setup capable of detecting individual quantum emitters in the blue and ultraviolet (UV) range. We demonstrate that the activation of individual B centers is spatially and temporally correlated with the deactivation of individual UV centers emitting at 4.1 eV, which are ubiquitous in hBN. We then make use of the ability to detect individual B center activation events to demonstrate the controlled creation of an array with only one emitter per irradiation site. Additionally, we demonstrate a symmetric technique for the heralded selective deactivation of individual emitters. Our results provide insights into the microscopic structure and activation mechanism of B centers, as well as versatile techniques for their deterministic integration.
在六方氮化硼(hBN)的各种量子发射体中,蓝色发射色中心或B中心由于其优异的量子光学性质而引起了人们的特别关注。此外,它们可以被电子束局部激活的事实使它们适合于自上而下集成到光子器件中。然而,由于缺乏对单个发射体敏感的实时监测技术,激活过程在发射体数量上是随机的,其机制也存在争议。在这里,我们实现了一个原位阴极发光监测装置,能够检测蓝色和紫外线(UV)范围内的单个量子发射器。我们证明了单个B中心的激活在空间和时间上与发射4.1 eV的单个UV中心的失活相关,这些中心在hBN中普遍存在。然后,我们利用检测单个B中心激活事件的能力来演示每个照射点只有一个发射器的阵列的受控创建。此外,我们还演示了一种对称技术,用于预告单个发射器的选择性失活。我们的研究结果提供了对B中心微观结构和激活机制的见解,以及对其确定性整合的通用技术。
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引用次数: 0
Light-Programmable Polyester Networks with Movable Cross-Links for On-Demand Enzymatic Degradation 轻型可编程聚酯网络与可移动的交联按需酶降解
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-25 DOI: 10.1021/acsnano.5c19646
Xin Zhou,Jiaxiong Liu,Kenji Yamaoka,Ryohei Ikura,Akihide Sugawara,Go Matsuba,Hiroshi Uyama,Yoshinori Takashima
The design of sustainable materials that integrates mechanical toughness with on-demand degradability remains a central challenge in the development of materials science. Here, we present a photoresponsive polyester capable of light-regulated enzymatic degradation through movable cross-links. The material consists of a poly(ε-caprolactone) backbone and inclusion complexes between photoisomerizable trans-stilbene (tSti) units and triacetylated γ-cyclodextrin (TAcγCD) units. Upon UV-A (λ = 350 nm) or UV-C (λ = 254 nm) irradiation, stilbene units undergo reversible trans–cis isomerization, repositioning cyclodextrin (CD) rings along the backbone and thereby switching the molecular coverage of enzyme-active ester groups. In the trans state, polyester segments are exposed, accelerating lipase-catalyzed degradation; in the cis state, ester groups are shielded, suppressing degradation. The switching is reversible under alternating UV-A/UV-C irradiation and absent in the linear control lacking movable rings, demonstrating that controllable CD positioning is essential for degradation control. This study introduces a molecular-coverage-based design rule that reconciles toughness and degradability for sustainable, environmentally benign polymers.
将机械韧性与随需降解性相结合的可持续材料的设计仍然是材料科学发展中的核心挑战。在这里,我们提出了一种光反应聚酯,能够通过可移动的交联进行光调节的酶降解。该材料由聚ε-己内酯骨架和光异构反式二苯乙烯(tSti)单元和三乙酰化γ-环糊精(tac - cd)单元之间的包合物组成。在UV-A (λ = 350 nm)或UV-C (λ = 254 nm)照射下,苯乙烯单元发生可逆的反顺异构化,环糊精(CD)环沿主干重新定位,从而改变酶活性酯基的分子覆盖范围。在反式状态下,聚酯片段暴露,加速脂肪酶催化降解;在顺式状态下,酯基被屏蔽,抑制降解。在UV-A/UV-C交替照射下,这种切换是可逆的,而在缺乏活动环的线性控制中则不存在,这表明可控的CD定位对降解控制至关重要。本研究介绍了一种基于分子覆盖率的设计规则,该规则可以协调可持续、环保聚合物的韧性和可降解性。
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引用次数: 0
Multifunctional Microneedle Patch with Antibacterial, Antioxidant, and Pro-Regenerative Properties for Scarless Wound Healing 具有抗菌、抗氧化和促进再生特性的多功能微针贴片,用于无疤痕伤口愈合
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-25 DOI: 10.1021/acsnano.6c01964
Guoqing Zhang, Miaomiao Wei, Zihan Zhang, Shixuan Chen, Wenbing Wan
Trauma can easily cause large-area skin tissue defects and is accompanied by bacterial infection, excessive oxidative stress, and unregulated inflammation, resulting in delayed healing and scar formation. This study presents a microneedle patch with a core–shell architecture, designed to address these challenges through integrated therapeutic functionalities. The shell of the microneedles incorporates melanin nanoparticles chelated with copper ions for controlling bacterial infection, and the core of the microneedles is filled with salvianolic acid B microparticles to reduce scar formation. In vitro analyses demonstrated the patch’s capacity to effectively eliminate reactive oxygen species (ROS), inhibit bacterial growth, and promote fibroblast migration and angiogenesis. Computational simulations further revealed its controlled drug diffusion, ensuring sustained therapeutic effects. In vivo experiments using S. aureus-infected wound models confirmed the patch’s efficacy in accelerating wound closure, reducing inflammation, and mitigating scar formation. Histopathological analysis and RNA sequencing highlighted its role in modulating inflammatory and collagen deposition pathways, while promoting balanced tissue regeneration. The microneedle system offers a promising platform for wound healing and scar prevention, combining targeted drug delivery with multifunctional therapeutic effects.
创伤容易造成大面积皮肤组织缺损,并伴有细菌感染、过度氧化应激和不调节的炎症,导致愈合延迟和瘢痕形成。本研究提出了一种具有核-壳结构的微针贴片,旨在通过综合治疗功能解决这些挑战。微针的外壳包含与铜离子螯合的黑色素纳米颗粒,用于控制细菌感染,微针的核心充满丹酚酸B微颗粒,以减少疤痕的形成。体外分析表明,该贴片能够有效消除活性氧(ROS),抑制细菌生长,促进成纤维细胞迁移和血管生成。计算模拟进一步揭示了其控制药物扩散,确保持续的治疗效果。利用金黄色葡萄球菌感染的伤口模型进行的体内实验证实了该贴片在加速伤口愈合、减少炎症和减轻疤痕形成方面的功效。组织病理学分析和RNA测序强调了其在调节炎症和胶原沉积途径中的作用,同时促进平衡的组织再生。微针系统结合靶向给药和多功能治疗效果,为伤口愈合和疤痕预防提供了一个有前景的平台。
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引用次数: 0
Dimensionality-Mixed Phases Facilitate Chirality Transfer and Spin-Orbit Coupling for Chiral Perovskite Red Spin-LEDs 维数混合相促进手性钙钛矿红自旋led的手性转移和自旋轨道耦合
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-25 DOI: 10.1021/acsnano.5c22124
Sheng Tao,Linze Jiang,Liqun Liu,Houzhi Chen,Jun Tang,Chao Qian,Peiran Fan,Lin Zhu,Pengxi Chen,Jin Zhou,Yang Qin,Xiangnan Sun,Hanlin Hu,Jing Li,Xixiang Zhu,Haomiao Yu,Yumeng Shi,Jinpeng Li,Zhi-gang Yu,Bin Hu,Kai Wang
Chiral hybrid perovskite spin-light emitting diodes (spin-LEDs) adopt spin filtration technology based on chirality-induced spin selectivity (CISS), while circularly polarized electroluminescence (CP-EL) arises from a direct conversion of spin angular momentum into light. The current obstacle lies in elevating the dissymmetry factors for circularly polarized luminescence in quasi-2D chiral-achiral synergistic systems. Herein, chiral organic ligands R-/S-methylbenzylamine (R-/S-MBA) were incorporated into lead-iodide octahedral inorganic frameworks, forming dimensional-mixing phases. An effective chirality transfer through the visible light region and chirality-induced spin–orbit coupling (CISOC) strengths of up to 0.8081 eV·Å were achieved for ultrathin red emitters. Without spin injection, prominent dissymmetry factors of CP-EL approaching 20% were obtained for R-/S-MBA-based bright red single-junction spin-LEDs. Our work greatly promotes the development high-performance red chiral perovskite spin-LEDs.
手性杂化钙钛矿自旋发光二极管(spin- leds)采用基于手性诱导自旋选择性(CISS)的自旋过滤技术,而圆极化电致发光(CP-EL)是由自旋角动量直接转化为光产生的。目前的障碍在于提高准二维手性-非手性协同体系圆极化发光的不对称因子。将手性有机配体R-/ s -甲基苄胺(R-/S-MBA)掺入碘化铅八面体无机框架中,形成尺度混合相。超薄红色发射体在可见光区实现了有效的手性转移,手性诱导自旋轨道耦合(CISOC)强度高达0.8081 eV·Å。在不注入自旋的情况下,R-/ s - mba基亮红色单结自旋led的CP-EL不对称系数接近20%。我们的工作极大地促进了高性能红手性钙钛矿自旋led的发展。
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引用次数: 0
Breaking Inversion Symmetry in 2D Semiconductors by Built-In Electric Fields across the van der Waals Metal–Semiconductor Interface 范德华金属-半导体界面内建电场破坏二维半导体中的反演对称性
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-25 DOI: 10.1021/acsnano.5c13154
Chuansheng Xia,Xinyu Yang,Qiannan Cui,Chaoyang Huang,Rui Wang,Yuanyuan Li,Xiaoxuan Wang,Bing Gu,Shuai Dong,Chunxiang Xu
As important building blocks of integrated optoelectronic chips, most multilayer and bulk 2D layered semiconductors undertake out-of-plane inversion symmetry, which limits their multifunctional applications. Here, we propose a facile interfacial engineering means of breaking such inversion symmetry by built-in electric fields across the semiconductor–metal van der Waals heterointerface. Broken inversion symmetry of 2H WS2 layers has been experimentally confirmed by strong second harmonic generation (SHG) in fabricated bulk WS2/Au heterostructures. Through correlated SHG, atomic force, and surface potential mapping measurements and density function theory simulation (DFT), we unambiguously confirm the proposed physical mechanism. These results provide more possibilities of utilizing a 2D semiconductor/metal heterostructure to construct multifunctional integrated optoelectronic chips.
作为集成光电芯片的重要组成部分,大多数多层和块状二维层状半导体存在面外反演对称性,限制了其多功能应用。在这里,我们提出了一种简单的界面工程方法,通过半导体-金属范德华异质界面上的内置电场来打破这种反转对称性。在制备的块体WS2/Au异质结构中,通过强二次谐波产生(SHG)实验证实了2H WS2层的破逆对称性。通过相关的SHG、原子力、表面电位映射测量和密度函数理论模拟(DFT),我们明确地证实了所提出的物理机制。这些结果为利用二维半导体/金属异质结构构建多功能集成光电芯片提供了更多的可能性。
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引用次数: 0
AI-Agent-Guided Design of Dual-Scale Modulated Nickel-Based Catalyst with Built-In Electric Field for Enhanced Biomass Electrooxidation 基于人工智能的内置电场双尺度调制镍基催化剂增强生物质电氧化的设计
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-25 DOI: 10.1021/acsnano.6c00124
Pengwei Zhao, Yefan Zhang, Bin Chen, Weipeng Zhao, Zhuo Chen, Linjie Guan, Shengzhenzhi Sun, Shuya Zhang, Yang Li, Wenchao Peng, Qicheng Zhang, Xiaobin Fan
Electrochemical synthesis offers a sustainable route for chemical production, and integrating artificial intelligence (AI) into electrocatalyst design promises to accelerate the development of efficient processes. Herein, we report an AI-agent-assisted strategy for the design of a nickel-based catalyst with a built-in electric field (BEF) for the electrooxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA). The AI-agent autonomously identified Mn doping as a means to create a BEF that simultaneously optimizes the electronic structure and the interfacial microenvironment. These synergistic effects enable the resulting Mn–Ni(OH)2 catalyst to achieve a current density exceeding 700 mA cm–2 at 1.45 V vs RHE, with HMF conversion, Faradaic efficiency, and FDCA selectivity all surpassing 99%. Notably, after 45 cycles, the activity of Mn–Ni(OH)2 remains stable. When assembled into a flow electrolyzer, current densities of 0.5 and 1 A cm–2 are achieved at cell voltages of 1.735 and 2.162 V, respectively, over a duration of 100 h. Characterization and simulation results reveal that the BEF enhances charge transfer by modulating the Ni eg* orbital and accelerates mass transport by disrupting the interfacial hydrogen-bond networks. This AI-assisted, dual-regulation strategy bridges the gap between catalyst electronic structure engineering and interfacial microenvironment design for sustainable electrosynthesis applications.
电化学合成为化工生产提供了一条可持续的途径,将人工智能(AI)集成到电催化剂设计中有望加速高效工艺的发展。在此,我们报告了一种ai试剂辅助策略,用于设计具有内置电场(BEF)的镍基催化剂,用于将5-羟甲基糠醛(HMF)电氧化为2,5-呋喃二羧酸(FDCA)。ai代理自主识别Mn掺杂作为创建同时优化电子结构和界面微环境的BEF的手段。这些协同效应使所得到的Mn-Ni (OH)2催化剂在1.45 V vs RHE下的电流密度超过700 mA cm-2, HMF转化率、法拉第效率和FDCA选择性均超过99%。值得注意的是,经过45次循环后,Mn-Ni (OH)2的活性保持稳定。当组装到流动电解槽中时,在1.735 V和2.162 V的电池电压下,电流密度分别达到0.5和1 a cm-2。表征和模拟结果表明,BEF通过调制Ni eg*轨道来增强电荷转移,并通过破坏界面氢键网络来加速质量传递。这种人工智能辅助的双调节策略弥合了催化剂电子结构工程和界面微环境设计之间的差距,以实现可持续的电合成应用。
{"title":"AI-Agent-Guided Design of Dual-Scale Modulated Nickel-Based Catalyst with Built-In Electric Field for Enhanced Biomass Electrooxidation","authors":"Pengwei Zhao, Yefan Zhang, Bin Chen, Weipeng Zhao, Zhuo Chen, Linjie Guan, Shengzhenzhi Sun, Shuya Zhang, Yang Li, Wenchao Peng, Qicheng Zhang, Xiaobin Fan","doi":"10.1021/acsnano.6c00124","DOIUrl":"https://doi.org/10.1021/acsnano.6c00124","url":null,"abstract":"Electrochemical synthesis offers a sustainable route for chemical production, and integrating artificial intelligence (AI) into electrocatalyst design promises to accelerate the development of efficient processes. Herein, we report an AI-agent-assisted strategy for the design of a nickel-based catalyst with a built-in electric field (BEF) for the electrooxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA). The AI-agent autonomously identified Mn doping as a means to create a BEF that simultaneously optimizes the electronic structure and the interfacial microenvironment. These synergistic effects enable the resulting Mn–Ni(OH)<sub>2</sub> catalyst to achieve a current density exceeding 700 mA cm<sup>–2</sup> at 1.45 V vs RHE, with HMF conversion, Faradaic efficiency, and FDCA selectivity all surpassing 99%. Notably, after 45 cycles, the activity of Mn–Ni(OH)<sub>2</sub> remains stable. When assembled into a flow electrolyzer, current densities of 0.5 and 1 A cm<sup>–2</sup> are achieved at cell voltages of 1.735 and 2.162 V, respectively, over a duration of 100 h. Characterization and simulation results reveal that the BEF enhances charge transfer by modulating the Ni e<sub>g</sub>* orbital and accelerates mass transport by disrupting the interfacial hydrogen-bond networks. This AI-assisted, dual-regulation strategy bridges the gap between catalyst electronic structure engineering and interfacial microenvironment design for sustainable electrosynthesis applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"4 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507478","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Simultaneous Monitoring of Cytochrome c and Caspase-3 Dynamics Using a Dual-Channel Nanoprobe for Deciphering Single-Cell Apoptosis. 使用双通道纳米探针同时监测细胞色素c和Caspase-3动力学,以破译单细胞凋亡。
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-24 DOI: 10.1021/acsnano.5c22623
Xinhao Li,Weikang Hu,Yao Huang,Yanmei Ma,Zuokun Yin,Tong Wang,Chengzhi Hu
Unraveling the precise kinetics of the intrinsic apoptotic pathway requires resolution of the temporal lag between mitochondrial permeabilization and downstream proteolytic execution. However, dissecting these distinct molecular events within the crowded cytosolic environment of a single live cell remains limited by the lack of nonperturbative, multiplexed sensing tools. Here, we report a dual-channel nanoprobe capable of label-free, simultaneous monitoring of Cytochrome c (Cyt c) translocation and Caspase-3 activation. The nanoprobe features physically isolated nanochannels allowing for orthogonal functionalization: one channel acts as an aptamer-based sensor for Cyt c, while the second functions via the enzymatic cleavage of a specific peptide substrate by Caspase-3. This design enables the synchronous transduction of protein binding and enzymatic activity into independent current signals. The probe exhibited high sensitivity, selectivity, and stability in complex biological fluids. We applied this platform to monitor the dynamics of Cyt c and caspase-3 in breast cancer cells, revealing significant heterogeneity in apoptosis and a spatiotemporal delay between Cyt c release and caspase-3 activation, consistent with the intrinsic apoptosis pathway. This dual-detection methodology provides a minimally invasive approach with high spatial and temporal resolution for probing apoptotic signaling at the single-cell level and enables quantitative assessment of heterogeneous cellular responses to apoptotic stimuli.
揭示内在凋亡途径的精确动力学需要解决线粒体渗透和下游蛋白水解执行之间的时间滞后。然而,在单个活细胞拥挤的细胞质环境中解剖这些不同的分子事件仍然受到缺乏非扰动、多路传感工具的限制。在这里,我们报道了一种双通道纳米探针,能够无标记地同时监测细胞色素c (Cyt c)易位和Caspase-3激活。纳米探针具有物理隔离的纳米通道,允许正交功能化:一个通道作为基于适体的Cyt c传感器,而第二个通道通过Caspase-3对特定肽底物的酶切发挥作用。这种设计使蛋白质结合和酶活性同步转导成独立的电流信号。该探针在复杂的生物流体中具有较高的灵敏度、选择性和稳定性。我们利用该平台监测乳腺癌细胞中Cyt - c和caspase-3的动态变化,发现细胞凋亡具有显著的异质性,Cyt - c释放和caspase-3激活之间存在时空延迟,与固有的细胞凋亡途径一致。这种双检测方法提供了一种具有高空间和时间分辨率的微创方法,用于在单细胞水平上探测凋亡信号,并能够定量评估细胞对凋亡刺激的异质反应。
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引用次数: 0
When Atoms Choose Their Neighbors: Element-Specific Views of Local Chemical Order in High-Entropy Alloys. 当原子选择它们的邻居:高熵合金中局部化学秩序的元素特定观点。
IF 16 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-24 Epub Date: 2026-03-09 DOI: 10.1021/acsnano.5c21782
David Morris, Yonggang Yao, Peng Zhang

Local chemical order (LCO) is a key descriptor linking composition, atomic arrangement, and function in high-entropy alloys (HEAs) yet remains difficult to quantify. This perspective highlights how X-ray absorption spectroscopy (XAS) provides element-specific, quantitative insight into LCO in complex alloys. We outline practical considerations for XAS data collection and fitting, including the width of spectra range, multitemperature analysis, and X-ray absorption edge choice for 5d elements. We then highlight a coordination-number-based framework for LCO analysis and use model HEAs to show how single-atom and near-single-atom motifs naturally emerge as component number increases, bridging HEAs and single-atom alloys. Finally, we identify priorities, including standardized protocols, uncertainty quantification, expanded operando and time-resolved XAS, and integration with complementary characterization and modeling.

局部化学顺序(LCO)是连接高熵合金(HEAs)的组成、原子排列和功能的关键描述子,但仍然难以量化。这一观点强调了x射线吸收光谱(XAS)如何为复杂合金中的LCO提供特定元素的定量洞察。我们概述了XAS数据收集和拟合的实际考虑因素,包括光谱范围的宽度,多温度分析和5d元素的x射线吸收边缘选择。然后,我们强调了基于配位数的LCO分析框架,并使用模型HEAs来显示单原子和近单原子基序如何随着组分数的增加而自然出现,将HEAs和单原子合金连接起来。最后,我们确定了优先事项,包括标准化协议、不确定性量化、扩展操作和时间分辨XAS,以及与互补表征和建模的集成。
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引用次数: 0
Valley-Dependent Emission Patterns Enabled by Plasmonic Nanoantennas. 等离子体纳米天线实现的谷相关发射模式。
IF 16 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-24 DOI: 10.1021/acsnano.5c11672
Tobias Bucher, Jingshi Yan, Jan Sperrhake, Zlata Fedorova, Mostafa Abasifard, Rajeshkumar Mupparapu, Haitao Chen, Emad Najafidehaghani, Khosro Zangeneh Kamali, Antony George, Mohsen Rahmani, Thomas Pertsch, Andrey Turchanin, Dragomir N Neshev, Isabelle Staude

Selective control of the emission pattern of valley-polarized excitons in monolayer transition metal dichalcogenides is essential for advancing valleytronic, quantum information, and optoelectronic devices. Although substantial progress has been made in directionally routing photoluminescence from these materials, key challenges persist: specifically, establishing how observed routing effects relate to the degree of valley polarization and distinguishing genuine valley-dependent routing from spin-momentum coupling, an optical scattering effect unrelated to the emitter. In this work, we address these challenges by experimentally and numerically demonstrating a direct link between excitonic valley polarization and the resulting farfield emission pattern, enabling quantitative evaluation of valley-selective emission routing. We report valley-dependent manipulation of the angular emission pattern of monolayer tungsten diselenide using gold nanobar dimer antennas at cryogenic temperatures. By probing the emission under opposite circularly polarized excitation, we observe a valley-selective asymmetry in the photoluminescence circular dichroism of 2%. These measurements are supported by a reciprocity-based numerical framework that enables modeling of valley-selective emission in periodic systems. Our calculations further reveal that the observed valley-dependent directionality is a symmetry-protected property of the nanoantenna array arising from its extrinsic chirality at oblique emission angles, and that it can be substantially enhanced by tailoring the emitter distribution. Together, these results establish our nanoantenna platform as a robust route toward valleytronic signal processing.

对单层过渡金属二硫族化合物中谷极化激子发射模式的选择性控制对于推进谷电子、量子信息和光电子器件的发展至关重要。尽管从这些材料中定向布线光致发光已经取得了实质性进展,但关键的挑战仍然存在:具体来说,建立观察到的布线效应与谷极化程度的关系,以及区分真正的谷依赖布线与自旋动量耦合,一种与发射器无关的光学散射效应。在这项工作中,我们通过实验和数值证明了激子谷极化与由此产生的远场发射模式之间的直接联系,从而能够定量评估谷选择发射路径,从而解决了这些挑战。我们报道了利用金纳米棒二聚体天线在低温下对单层二硒化钨的角发射模式的谷依赖操纵。通过探测圆偏振激发下的发射,我们观察到光致发光圆二色性为2%时存在谷选择不对称性。这些测量是由一个基于往复的数值框架支持的,该框架使周期性系统中的谷选择性发射建模成为可能。我们的计算进一步揭示了观测到的谷相关方向性是纳米天线阵列的对称性保护特性,这是由其在斜发射角处的外在手性引起的,并且可以通过调整发射极分布来大大增强。总之,这些结果使我们的纳米天线平台成为谷电子信号处理的可靠途径。
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引用次数: 0
Molecular Views of Mineral Carbonation: Reaction of CO2 with the Wollastonite (100) Surface 矿物碳酸化的分子观点:CO2与硅灰石(100)表面的反应
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-03-24 DOI: 10.1021/acsnano.5c19629
Andrea Conti,Luca Lezuo,Alexander Hoheneder,Elena Vaníčková,Domitilla Alessandra Aloi,Andreas Steiger-Thirsfeld,David Heuser,Rainer Abart,Florian Mittendorfer,Michael Schmid,Ulrike Diebold,Giada Franceschi
The carbonation of silicate minerals is a key process in the Earth’s carbon cycle and offers a promising avenue for long-term CO2 sequestration. However, the atomistic mechanisms by which CO2 is activated at silicate surfaces remain poorly understood, largely due to the intrinsic complexity and insulating nature of these materials. To close this gap, wollastonite (CaSiO3) is used as a model system. Noncontact atomic force microscopy (nc-AFM) with functionalized tips is combined with density functional theory (DFT) to investigate its lowest-energy (100) surface under ultrahigh vacuum (UHV). Upon cleaving the mineral in UHV, water vapor is released from the sample and spontaneously readsorbs into a previously unreported, exceptionally stable configuration. The resulting surface hydration layer promotes spontaneous CO2 chemisorption and the formation of surface carbonates with negligible kinetic barriers. Our results offer atomic-scale evidence of gas–phase carbonation on a silicate mineral, revealing a water-assisted pathway for CO2 capture that bypasses aqueous mineral dissolution.
硅酸盐矿物的碳酸化是地球碳循环的关键过程,为长期封存二氧化碳提供了一条有希望的途径。然而,二氧化碳在硅酸盐表面被激活的原子机制仍然知之甚少,这主要是由于这些材料的内在复杂性和绝缘性。为了弥补这一差距,硅灰石(CaSiO3)被用作模型体系。将功能化尖端的非接触原子力显微镜(nc-AFM)与密度泛函理论(DFT)相结合,研究了超高真空(UHV)下其最低能量(100)表面。在特高压下切割矿物时,水蒸气从样品中释放出来,并自发地重新吸收成以前未报道过的异常稳定的结构。由此产生的表面水化层促进自发的CO2化学吸附和表面碳酸盐的形成,其动力学障碍可以忽略不计。我们的研究结果为硅酸盐矿物的气相碳酸化提供了原子尺度的证据,揭示了一种水辅助的二氧化碳捕获途径,绕过了水矿物溶解。
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引用次数: 0
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