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Unravelling the Ageing Effects of PDMS-Based Triboelectric Nanogenerators (Adv. Mater. Interfaces 19/2024) 揭示基于 PDMS 的三电纳米发电机的老化效应(Adv.)
IF 4.3 3区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-05 DOI: 10.1002/admi.202470049
Tianhuai Xu, Jiahao Ye, Jin-Chong Tan

Triboelectricity

PDMS-based triboelectric nanogenerator (TENG) under nanoscale investigation, employing a scanning near-field optical microscope. A conductive probe mounted at the end of the cantilever generates nanofocus for incident infrared irradiation, scattered light reveals the surface chemical properties of the pristine versus aged PDMS films. Breakage of SiO bonds results in the chain scission process that will degrade TENG performance. More details can be found in article 2400094 by Jin-Chong Tan and co-workers.

使用扫描近场光学显微镜对基于 PDMS 的三电纳米发电机 (TENG) 进行纳米级研究。安装在悬臂末端的导电探针产生纳米焦点,用于入射红外线照射,散射光揭示了原始 PDMS 薄膜和老化 PDMS 薄膜的表面化学特性。SiO 键的断裂会导致链裂过程,从而降低 TENG 的性能。更多详情,请参阅 Jin-Chong Tan 及其合作者撰写的文章 2400094。
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引用次数: 0
Advanced Nanocarbons Toward two-Electron Oxygen Electrode Reactions for H2O2 Production and Integrated Energy Conversion. 用于 H2O2 生产和综合能源转换的双电子氧电极反应的先进纳米碳。
IF 13 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-05 DOI: 10.1002/smll.202403029
Linjie Zhao, Riqing Yan, Baoguang Mao, Rajib Paul, Wenjie Duan, Liming Dai, Chuangang Hu

Hydrogen peroxide (H2O2) plays a pivotal role in advancing sustainable technologies due to its eco-friendly oxidizing capability. The electrochemical two-electron (2e-) oxygen reduction reaction and water oxidation reaction present an environmentally green method for H2O2 production. Over the past three years, significant progress is made in the field of carbon-based metal-free electrochemical catalysts (C-MFECs) for low-cost and efficient production of H2O2 (H2O2EP). This article offers a focused and comprehensive review of designing C-MFECs for H2O2EP, exploring the construction of dual-doping configurations, heteroatom-defect coupling sites, and strategic dopant positioning to enhance H2O2EP efficiency; innovative structural tuning that improves interfacial reactant concentration and promote the timely release of H2O2; modulation of electrolyte and electrode interfaces to support the 2e- pathways; and the application of C-MFECs in reactors and integrated energy systems. Finally, the current challenges and future directions in this burgeoning field are discussed.

过氧化氢(H2O2)具有环保的氧化能力,在推动可持续技术发展方面发挥着举足轻重的作用。电化学双电子(2e-)氧还原反应和水氧化反应是一种生产 H2O2 的环保方法。过去三年来,用于低成本高效生产 H2O2(H2O2EP)的碳基无金属电化学催化剂(C-MFECs)领域取得了重大进展。本文对设计用于 H2O2EP 的碳基无金属电化学催化剂(C-MFECs)进行了重点而全面的综述,探讨了如何构建双掺杂配置、杂原子-缺陷耦合位点以及战略性掺杂定位来提高 H2O2EP 的效率;如何进行创新性结构调整以提高界面反应物浓度并促进 H2O2 的及时释放;如何调节电解质和电极界面以支持 2e- 途径;以及如何将 C-MFECs 应用于反应器和集成能源系统。最后,还讨论了这一新兴领域目前面临的挑战和未来的发展方向。
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引用次数: 0
Electron-Delocalization Across High Surface Entropy Sub-1 nm Nanobelts Toward Enhanced Electrocatalytic Urea Oxidation. 高表面熵 1 纳米以下纳米颗粒上的电子定位,促进电催化尿素氧化。
IF 13 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-05 DOI: 10.1002/smll.202404595
Xijun Cheng, Siyang Nie, Yuan Huang, Qingda Liu, Liang Wu, Xun Wang

Integration of inherently incompatible elements into a single sublattice, resulting in the formation of monophasic metal oxide, holds great scientific promise; it unveils that the overlooked surface entropy in subnanometer materials can thermodynamically facilitate the formation of homogeneous single-phase structures. Here a facile approach is proposed for synthesizing multimetallic oxide subnanometer nanobelts (MMO-PMA SNBs) by harnessing the potential of phosphomolybdic acid (PMA) clusters to capture inorganic nuclei and inhibiting their subsequent growth in solvothermal reactions. Experimental and theoretical analyses show that PMA in MMO-PMA SNBs not only aids subnanometer structure formation but also induces in situ modifications to catalytic sites. The electron transfer from PMA, coupled with the loss of elemental identity of transition metals, leads to electron delocalization, jointly activating the reaction sites. The unique structure makes pentametallic oxide (PMO-PMA SNBs) achieve a current density of 10 mA cm-2 at a low potential of 1.34 V and remain stable for 24 h at 10 mA cm-2 on urea oxidation reaction (UOR). The exceptional UOR catalytic activity suggests a potential for utilizing multimetallic subnanometer nanostructures in energy conversion and environmental remediation.

将本质上不相容的元素整合到一个单一的亚晶格中,形成单相金属氧化物,具有巨大的科学前景;它揭示了亚纳米材料中被忽视的表面熵可以在热力学上促进均匀单相结构的形成。本文提出了一种简便的方法,通过利用磷钼酸(PMA)团簇捕获无机核的潜力,抑制它们在溶热反应中的后续生长,从而合成多金属氧化物亚纳米颗粒(MMO-PMA SNBs)。实验和理论分析表明,MMO-PMA SNB 中的 PMA 不仅有助于亚纳米结构的形成,还能诱导催化位点的原位修饰。PMA 的电子转移以及过渡金属元素特性的丧失导致了电子析出,从而共同激活了反应位点。这种独特的结构使得五金属氧化物(PMO-PMA SNBs)在 1.34 V 的低电位下电流密度达到 10 mA cm-2,并在 10 mA cm-2 的尿素氧化反应(UOR)中保持稳定 24 小时。卓越的尿素氧化反应催化活性表明,多金属亚纳米结构在能源转换和环境修复方面具有广阔的应用前景。
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引用次数: 0
Spatially Dependent in-Gap States Induced by Andreev Tunneling through a Single Electronic State. 安德烈耶夫隧道穿越单一电子态诱导的空间相关隙内态
IF 9.6 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-05 DOI: 10.1021/acs.nanolett.4c01581
Ruixia Zhong, Zhongzheng Yang, Qi Wang, Fanbang Zheng, Wenhui Li, Juefei Wu, Chenhaoping Wen, Xi Chen, Yanpeng Qi, Shichao Yan

By using low-temperature scanning tunneling microscopy and spectroscopy (STM/STS), we observe in-gap states induced by Andreev tunneling through a single impurity state in a low carrier density superconductor (NaAlSi). The energy-symmetric in-gap states appear when the impurity state is located within the superconducting gap. In-gap states can cross the Fermi level, and they show X-shaped spatial variation. We interpret the in-gap states as a consequence of the Andreev tunneling through the impurity state, which involves the formation or breakup of a Cooper pair. Due to the low carrier density in NaAlSi, the in-gap state is tunable by controlling the STM tip-sample distance. Under strong external magnetic fields, the impurity state shows Zeeman splitting when it is located near the Fermi level. Our findings not only demonstrate the Andreev tunneling involving single electronic state but also provide new insights for understanding the spatially dependent in-gap states in low carrier density superconductors.

通过使用低温扫描隧道显微镜和光谱学(STM/STS),我们在低载流子密度超导体(NaAlSi)中观察到了安德烈耶夫隧道通过单一杂质态诱导的隙内态。当杂质态位于超导间隙内时,就会出现能量对称的内隙态。内隙态可以跨越费米级,并呈现出 X 型空间变化。我们将这些内隙态解释为安德烈耶夫隧穿杂质态的结果,其中涉及库珀对的形成或断裂。由于 NaAlSi 中的载流子密度较低,因此可通过控制 STM 尖端与样品的距离来调整内隙态。在强外部磁场作用下,杂质态位于费米级附近时会出现泽曼分裂。我们的发现不仅证明了涉及单电子态的安德烈耶夫隧道现象,而且为理解低载流子密度超导体中空间依赖性内隙态提供了新的见解。
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引用次数: 0
Flotation Coefficient Distributions of Lipid Nanoparticles by Sedimentation Velocity Analytical Ultracentrifugation. 沉降速度分析超速离心法测定脂质纳米颗粒的浮选系数分布
IF 15.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-05 DOI: 10.1021/acsnano.4c05322
Huaying Zhao, Alioscka A Sousa, Peter Schuck

The robust characterization of lipid nanoparticles (LNPs) encapsulating therapeutics or vaccines is an important and multifaceted translational problem. Sedimentation velocity analytical ultracentrifugation (SV-AUC) has proven to be a powerful approach in the characterization of size-distribution, interactions, and composition of various types of nanoparticles across a large size range, including metal nanoparticles (NPs), polymeric NPs, and also nucleic acid loaded viral capsids. Similar potential of SV-AUC can be expected for the characterization of LNPs, but is hindered by the flotation of LNPs being incompatible with common sedimentation analysis models. To address this gap, we developed a high-resolution, diffusion-deconvoluted sedimentation/flotation distribution analysis approach analogous to the most widely used sedimentation analysis model c(s). The approach takes advantage of independent measurements of the average particle size or diffusion coefficient, which can be conveniently determined, for example, by dynamic light scattering (DLS). We demonstrate the application to an experimental model of extruded liposomes as well as a commercial LNP product and discuss experimental potential and limitations of SV-AUC. The method is implemented analogously to the sedimentation models in the free, widely used SEDFIT software.

对封装治疗药物或疫苗的脂质纳米颗粒(LNPs)进行可靠的表征是一个重要的、多方面的转化问题。沉降速度分析超速离心法(SV-AUC)已被证明是表征各种类型纳米颗粒(包括金属纳米颗粒 (NPs)、聚合物 NPs 和负载核酸的病毒外壳)在大尺寸范围内的尺寸分布、相互作用和组成的有力方法。SV-AUC 在表征 LNPs 方面也有类似的潜力,但由于 LNPs 的浮选与常见的沉降分析模型不兼容而受到阻碍。为了弥补这一缺陷,我们开发了一种高分辨率、扩散去卷积沉积/浮选分布分析方法,类似于最广泛使用的沉积分析模型 c(s)。该方法利用了平均粒径或扩散系数的独立测量值,这些测量值可以通过动态光散射(DLS)等方法方便地确定。我们演示了挤压脂质体实验模型和商用 LNP 产品的应用,并讨论了 SV-AUC 的实验潜力和局限性。该方法的实现类似于广泛使用的免费 SEDFIT 软件中的沉降模型。
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引用次数: 0
Next-Generation Green Hydrogen: Progress and Perspective from Electricity, Catalyst to Electrolyte in Electrocatalytic Water Splitting. 下一代绿色氢能:从电力、电催化水分离中的催化剂到电解质的进展与展望》。
IF 26.6 1区 材料科学 Q1 Engineering Pub Date : 2024-07-05 DOI: 10.1007/s40820-024-01424-2
Xueqing Gao, Yutong Chen, Yujun Wang, Luyao Zhao, Xingyuan Zhao, Juan Du, Haixia Wu, Aibing Chen

Green hydrogen from electrolysis of water has attracted widespread attention as a renewable power source. Among several hydrogen production methods, it has become the most promising technology. However, there is no large-scale renewable hydrogen production system currently that can compete with conventional fossil fuel hydrogen production. Renewable energy electrocatalytic water splitting is an ideal production technology with environmental cleanliness protection and good hydrogen purity, which meet the requirements of future development. This review summarizes and introduces the current status of hydrogen production by water splitting from three aspects: electricity, catalyst and electrolyte. In particular, the present situation and the latest progress of the key sources of power, catalytic materials and electrolyzers for electrocatalytic water splitting are introduced. Finally, the problems of hydrogen generation from electrolytic water splitting and directions of next-generation green hydrogen in the future are discussed and outlooked. It is expected that this review will have an important impact on the field of hydrogen production from water.

作为一种可再生能源,电解水产生的绿色氢气已引起广泛关注。在几种制氢方法中,它已成为最有前途的技术。然而,目前还没有一种大规模的可再生制氢系统能与传统的化石燃料制氢相媲美。可再生能源电催化分水制氢是一种理想的制氢技术,具有环保清洁、氢气纯度高的特点,符合未来发展的要求。本综述从电力、催化剂和电解质三个方面总结和介绍了水分裂制氢的现状。特别介绍了电催化分水制氢的关键电源、催化材料和电解槽的现状和最新进展。最后,讨论并展望了电解水分裂制氢的问题和下一代绿色氢气的未来发展方向。预计本综述将对水制氢领域产生重要影响。
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引用次数: 0
Organic Cations Texture Zinc Metal Anodes for Deep Cycling Aqueous Zinc Batteries. 用于深循环锌水电池的有机阳离子质地锌金属阳极。
IF 27.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-05 DOI: 10.1002/adma.202408287
Guoqiang Ma, Wentao Yuan, Xiaotong Li, Tongqiang Bi, Linhuan Niu, Yue Wang, Mengyu Liu, Yuanyuan Wang, Zhaoxi Shen, Ning Zhang

Manipulating the crystallographic orientation of zinc (Zn) metal to expose more (002) planes is promising to stabilize Zn anodes in aqueous electrolytes. However, there remain challenges involving the non-epitaxial electrodeposition of highly (002) textured Zn metal and the maintenance of (002) texture under deep cycling conditions. Herein, a novel organic imidazolium cations-assisted non-epitaxial electrodeposition strategy to texture electrodeposited Zn metals is developed. Taking the 1-butyl-3-methylimidazolium cation (Bmim+) as a paradigm additive, the as-prepared Zn film ((002)-Zn) manifests a compact structure and a highly (002) texture without containing (100) signal. Mechanistic studies reveal that Bmim+ featuring oriented adsorption on the Zn-(002) plane can reduce the growth rate of (002) plane to render the final exposure of (002) texture, and homogenize Zn nucleation and suppress H2 evolution to enable the compact electrodeposition. In addition, the formulated Bmim+-containing ZnSO4 electrolyte effectively sustains the (002) texture even under deep cycling conditions. Consequently, the combination of (002) texture and Bmim+-containing electrolyte endows the (002)-Zn electrode with superior cycling stability over 350 h under 20 mAh cm-2 with 72.6% depth-of-discharge, and assures the stable operation of full Zn batteries with both coin-type and pouch-type configurations, significantly outperforming the (002)-Zn and commercial Zn-based batteries in Bmim+-free electrolytes.

操纵锌(Zn)金属的结晶取向以暴露更多 (002) 平面有望在水性电解质中稳定锌阳极。然而,在非外延电沉积高(002)纹理锌金属以及在深度循环条件下保持(002)纹理方面仍然存在挑战。在此,我们开发了一种新型有机咪唑阳离子辅助的非外延电沉积策略,用于电沉积锌金属的纹理。以 1-丁基-3-甲基咪唑阳离子(Bmim+)为示例添加剂,制备的 Zn 薄膜((002)-Zn)结构紧凑,具有高度(002)纹理,不含(100)信号。机理研究发现,Bmim+ 在 Zn-(002)面上的定向吸附特性可降低(002)面的生长速度,使最终呈现(002)纹理,并使 Zn 成核均匀化,抑制 H2 的演化,从而实现紧凑的电沉积。此外,即使在深度循环条件下,所配制的含 Bmim+ 的 ZnSO4 电解液也能有效地维持(002)纹理。因此,(002)纹理和含 Bmim+ 电解质的结合使(002)-Zn 电极在 20 mAh cm-2 和 72.6% 放电深度条件下具有 350 小时以上的超强循环稳定性,并确保了硬币型和袋装型全 Zn 电池的稳定运行,其性能明显优于不含 Bmim+ 电解质的(002)-Zn 电池和商用 Zn 电池。
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引用次数: 0
Surface Engineering Enhances Vanadium Carbide MXene-Based Nanoplatform Triggered by NIR-II for Cancer Theranostics. 表面工程增强了由近红外-II 触发的碳化钒 MXene 型纳米平台,可用于癌症治疗。
IF 13 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-05 DOI: 10.1002/smll.202401655
Xiaodong Zhu, Xide Zhang, Jiahao Guo, Lei He, Fuming Wang, Zhiwen Qiu, Ang Li, Jing Zhang, Fu Gao, Wei Li

Despite the advantages of high tissue penetration depth, selectivity, and non-invasiveness of photothermal therapy for cancer treatment, developing NIR-II photothermal agents with desirable photothermal performance and advanced theranostics ability remains a key challenge. Herein, a universal surface modification strategy is proposed to effectively improve the photothermal performance of vanadium carbide MXene nanosheets (L-V2C) with the removal of surface impurity ions and generation of mesopores. Subsequently, MnOx coating capable of T1-weighted magnetic resonance imaging can be in situ formed through surface redox reaction on L-V2C, and then, stable nanoplatforms (LVM-PEG) under physiological conditions can be obtained after further PEGylation. In the tumor microenvironment irradiated by NIR-II laser, multivalent Mn ions released from LVM-PEG, as a reversible electronic station, can consume the overexpression of glutathione and catalyze a Fenton-like reaction to produce ·OH, resulting in synchronous cellular oxidative damage. Efficient synergistic therapy promotes immunogenic cell death, improving tumor-related immune microenvironment and immunomodulation, and thus, LVM-PEG can demonstrate high accuracy and excellent anticancer efficiency guided by multimodal imaging. As a result, this study provides a new approach for the customization of 2D surface strategies and the study of synergistic therapy mechanisms, highlighting the application of MXene-based materials in the biomedical field.

尽管光热疗法在癌症治疗中具有组织穿透深度高、选择性强和无创等优点,但开发具有理想光热性能和先进治疗能力的近红外-II光热制剂仍是一项关键挑战。本文提出了一种通用的表面改性策略,通过去除碳化钒 MXene 纳米片(L-V2C)表面杂质离子和生成介孔,有效提高其光热性能。随后,通过表面氧化还原反应在 L-V2C 上原位形成可进行 T1 加权磁共振成像的 MnOx 涂层,再经过 PEG 化处理,可获得生理条件下稳定的纳米平台(LVM-PEG)。在 NIR-II 激光照射下的肿瘤微环境中,LVM-PEG 释放的多价锰离子作为可逆电子站,可消耗过量表达的谷胱甘肽,并催化 Fenton 类反应产生 -OH,导致细胞同步氧化损伤。高效的协同治疗可促进免疫原性细胞死亡,改善肿瘤相关的免疫微环境和免疫调节,因此,LVM-PEG 可在多模态成像的指导下显示出高精度和卓越的抗癌效率。因此,本研究为二维表面策略的定制和协同治疗机制的研究提供了一种新方法,凸显了 MXene 基材料在生物医学领域的应用。
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引用次数: 0
Cell Membrane Engineered Polypeptide Nanonets Mimicking Macrophage Aggregates for Enhanced Antibacterial Treatment. 模仿巨噬细胞聚集体的细胞膜工程多肽纳米网,用于增强抗菌治疗。
IF 13 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-05 DOI: 10.1002/smll.202401845
Jiang Xiao, Zhongquan Song, Tengfei Liu, Zengchao Guo, Xiaohui Liu, Hui Jiang, Xuemei Wang

Drug-resistant bacterial infections and their lipopolysaccharide-related inflammatory complications continue to pose significant challenges in traditional treatments. Inspired by the rapid initiation of resident macrophages to form aggregates for efficient antibacterial action, this study proposes a multifunctional and enhanced antibacterial strategy through the construction of novel biomimetic cell membrane polypeptide nanonets (R-DPB-TA-Ce). The design involves the fusion of end-terminal lipidated polypeptides containing side-chain cationic boronic acid groups (DNPLBA) with cell membrane intercalation engineering (R-DPB), followed by coordination with the tannic acid-cerium complex (TA-Ce) to assemble into a biomimetic nanonet through boronic acid-polyphenol-metal ion interactions. In addition to the ability of RAW 264.7 macrophages cell membrane components' (R) ability to neutralize lipopolysaccharide (LPS), R-DPB-TA-Ce demonstrated enhanced capture of bacteria and its LPS, leveraging nanoconfinement-enhanced multiple interactions based on the boronic acid-polyphenol nanonets skeleton combined with polysaccharide. Utilizing these advantages, indocyanine green (ICG) is further employed as a model drug for delivery, showcasing the exceptional treatment effect of R-DPB-TA-Ce as a new biomimetic assembled drug delivery system in antibacterial, anti-inflammatory, and wound healing promotion. Thus, this strategy of mimicking macrophage aggregates is anticipated to be further applicable to various types of cell membrane engineering for enhanced antibacterial treatment.

耐药性细菌感染及其与脂多糖相关的炎症并发症仍然是传统治疗方法面临的重大挑战。受驻留巨噬细胞迅速形成聚集体以达到高效抗菌作用的启发,本研究通过构建新型仿生物细胞膜多肽纳米网(R-DPB-TA-Ce),提出了一种多功能增强型抗菌策略。该设计包括将含有侧链阳离子硼酸基团(DNPLBA)的末端脂化多肽与细胞膜插层工程(R-DPB)融合,然后与单宁酸铈复合物(TA-Ce)配位,通过硼酸-多酚-金属离子的相互作用组装成仿生纳米网。除了 RAW 264.7 巨噬细胞细胞膜成分(R)中和脂多糖(LPS)的能力外,R-DPB-TA-Ce 还利用基于硼酸-多酚纳米网骨架与多糖结合的纳米膦强化多重相互作用,增强了对细菌及其 LPS 的捕获能力。利用这些优势,吲哚菁绿(ICG)被进一步用作给药模型,展示了 R-DPB-TA-Ce 作为一种新型仿生组装给药系统在抗菌、消炎和促进伤口愈合方面的卓越治疗效果。因此,这种模拟巨噬细胞聚集体的策略有望进一步应用于各类细胞膜工程,以增强抗菌治疗效果。
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引用次数: 0
Interplay of Cooper Pairs and Zero-Energy Quasiparticles in a Gapless Superconductor. 无间隙超导体中库珀对与零能准粒子的相互作用
IF 27.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-05 DOI: 10.1002/adma.202404708
Jhinhwan Lee, Hae-Ryong Park, Jun Sung Kim, Han Woong Yeom

The interplay between Cooper pairs and Bogoliubov-de Gennes (BdG) quasiparticles is a topic of considerable interest in the quantum properties of solids, but its important ingredient, the sufficient amount of low-energy quasiparticles to interact with Cooper pairs remains elusive in conventional superconductors. Here a gapless superconductor with coupled paramagnetic atomic layers is used to generate a significant amount of zero-energy quasiparticles that Anderson-localize and bifurcate into regions of high and low zero-energy quasiparticle density of states. The enriched zero-energy quasiparticles induce puddled superconductivity and Josephson vortices. This discovery not only advances the understanding of the mutual interaction of Cooper pairs and BdG quasiparticles but also opens a new avenue for exploring and controlling exotic quantum phenomena where superconductivity, disorder, and spin degrees of freedom are entangled.

库珀对与波哥留布夫-德-吉尼斯(BdG)准粒子之间的相互作用是固体量子特性中一个颇受关注的话题,但其重要成分--与库珀对相互作用的足够数量的低能准粒子--在传统超导体中仍然难以捉摸。在这里,我们利用具有耦合顺磁原子层的无间隙超导体来产生大量零能准粒子,这些零能准粒子会发生安德森定位,并分叉成高零能和低零能准粒子态密度区域。富集的零能准粒子会诱发坑状超导和约瑟夫森漩涡。这一发现不仅加深了人们对库珀对和 BdG 准粒子相互影响的理解,而且为探索和控制超导性、无序性和自旋自由度纠缠在一起的奇异量子现象开辟了一条新途径。
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引用次数: 0
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