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Moving microscopic objects with self-disassembly 利用自组装技术移动微型物体
IF 38.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-31 DOI: 10.1038/s41565-024-01740-z
David B. Amabilino
Etching supramolecular fibres causes nanoscale motion of an attached bead from the etched end towards the middle of the fibre.
对超分子纤维进行蚀刻会导致附着的珠子从蚀刻端向纤维中部进行纳米级运动。
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引用次数: 0
Polymersomes with splenic avidity target red pulp myeloid cells for cancer immunotherapy 具有脾脏亲和性的聚合体靶向红髓髓细胞,用于癌症免疫疗法
IF 38.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-31 DOI: 10.1038/s41565-024-01727-w
Annelies C. Wauters, Jari F. Scheerstra, Mandy M. T. van Leent, Abraham J. P. Teunissen, Bram Priem, Thijs J. Beldman, Nils Rother, Raphaël Duivenvoorden, Geoffrey Prévot, Jazz Munitz, Yohana C. Toner, Jeroen Deckers, Yuri van Elsas, Patricia Mora-Raimundo, Gal Chen, Sheqouia A. Nauta, Anna Vera D. Verschuur, Arjan W. Griffioen, David P. Schrijver, Tom Anbergen, Yudong Li, Hanglong Wu, Alexander F. Mason, Marleen H. M. E. van Stevendaal, Ewelina Kluza, Richard A. J. Post, Leo A. B. Joosten, Mihai G. Netea, Claudia Calcagno, Zahi A. Fayad, Roy van der Meel, Avi Schroeder, Loai K. E. A. Abdelmohsen, Willem J. M. Mulder, Jan C. M. van Hest
Regulating innate immunity is an emerging approach to improve cancer immunotherapy. Such regulation requires engaging myeloid cells by delivering immunomodulatory compounds to hematopoietic organs, including the spleen. Here we present a polymersome-based nanocarrier with splenic avidity and propensity for red pulp myeloid cell uptake. We characterized the in vivo behaviour of four chemically identical yet topologically different polymersomes by in vivo positron emission tomography imaging and innovative flow and mass cytometry techniques. Upon intravenous administration, relatively large and spherical polymersomes accumulated rapidly in the spleen and efficiently targeted myeloid cells in the splenic red pulp. When loaded with β-glucan, intravenously administered polymersomes significantly reduced tumour growth in a mouse melanoma model. We initiated our nanotherapeutic’s clinical translation with a biodistribution study in non-human primates, which revealed that the platform’s splenic avidity is preserved across species. Delivering immunomodulatory compounds to myeloid cells can activate innate immunity for cancer immunotherapy. Here the authors design a polymersome-based nanocarrier for delivering β-glucan to red pulp myeloid cells in the spleen and show that their strategy achieves tumour growth reduction in a melanoma model.
调节先天性免疫是改善癌症免疫疗法的一种新兴方法。这种调节需要通过向包括脾脏在内的造血器官输送免疫调节化合物来吸引髓系细胞。在这里,我们介绍了一种基于聚合物组的纳米载体,它具有脾脏亲和性和红髓髓系细胞摄取倾向。我们通过体内正电子发射断层扫描成像以及创新的流式和质谱技术,对四种化学性质相同但拓扑结构不同的聚合体的体内行为进行了表征。静脉给药后,相对较大的球形聚合体在脾脏中迅速聚集,并有效靶向脾脏红髓中的髓样细胞。当载入β-葡聚糖时,静脉注射聚合体可显著减少小鼠黑色素瘤模型中的肿瘤生长。我们通过在非人灵长类动物中进行生物分布研究,启动了纳米疗法的临床转化。
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引用次数: 0
Co-transcriptional production of programmable RNA condensates and synthetic organelles 通过转录生产可编程 RNA 凝聚物和合成细胞器
IF 38.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-30 DOI: 10.1038/s41565-024-01726-x
Giacomo Fabrini, Nada Farag, Sabrina Pia Nuccio, Shiyi Li, Jaimie Marie Stewart, Anli A. Tang, Reece McCoy, Róisín M. Owens, Paul W. K. Rothemund, Elisa Franco, Marco Di Antonio, Lorenzo Di Michele
Condensation of RNA and proteins is central to cellular functions, and the ability to program it would be valuable in synthetic biology and synthetic cell science. Here we introduce a modular platform for engineering synthetic RNA condensates from tailor-made, branched RNA nanostructures that fold and assemble co-transcriptionally. Up to three orthogonal condensates can form simultaneously and selectively accumulate fluorophores through embedded fluorescent light-up aptamers. The RNA condensates can be expressed within synthetic cells to produce membrane-less organelles with a controlled number and relative size, and showing the ability to capture proteins using selective protein-binding aptamers. The affinity between otherwise orthogonal nanostructures can be modulated by introducing dedicated linker constructs, enabling the production of bi-phasic RNA condensates with a prescribed degree of interphase mixing and diverse morphologies. The in situ expression of programmable RNA condensates could underpin the spatial organization of functionalities in both biological and synthetic cells. Controlling RNA and protein condensation is helpful in synthetic biology. Here the authors show programmable assembly of synthetic RNA nanostructures into designer membrane-less organelles that selectively recruit ligands via protein-binding aptamers.
RNA 和蛋白质的凝结是细胞功能的核心,对其进行编程的能力在合成生物学和合成细胞科学中非常重要。在这里,我们介绍了一个模块化平台,用于从量身定制的支化 RNA 纳米结构中设计合成 RNA 缩合物,这些 RNA 纳米结构可通过转录进行折叠和组装。最多可同时形成三个正交凝聚体,并通过嵌入的荧光发光适配体选择性地积聚荧光团。RNA 缩聚物可以在合成细胞中表达,产生数量和相对大小可控的无膜细胞器,并显示出利用选择性蛋白质结合适配体捕获蛋白质的能力。通过引入专用的连接构建物,可以调节原本正交的纳米结构之间的亲和力,从而生产出具有规定相间混合程度和不同形态的双相 RNA 凝聚体。可编程 RNA 凝聚物的原位表达可为生物细胞和合成细胞的功能空间组织提供支持。
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引用次数: 0
A modular DNA origami nanocompartment for engineering a cell-free, protein unfolding and degradation pathway 用于设计无细胞蛋白质展开和降解途径的模块化 DNA 折纸纳米隔室
IF 38.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-29 DOI: 10.1038/s41565-024-01738-7
J. Huang, A. Jaekel, J. van den Boom, D. Podlesainski, M. Elnaggar, A. Heuer-Jungemann, M. Kaiser, H. Meyer, B. Saccà
Within the cell, chemical reactions are often confined and organized through a modular architecture. This facilitates the targeted localization of molecular species and their efficient translocation to subsequent sites. Here we present a cell-free nanoscale model that exploits compartmentalization strategies to carry out regulated protein unfolding and degradation. Our synthetic model comprises two connected DNA origami nanocompartments (each measuring 25 nm × 41 nm × 53 nm): one containing the protein unfolding machine, p97, and the other housing the protease chymotrypsin. We achieve the unidirectional immobilization of p97 within the first compartment, establishing a gateway mechanism that controls substrate recruitment, translocation and processing within the second compartment. Our data show that, whereas spatial confinement increases the rate of the individual reactions by up to tenfold, the physical connection of the compartmentalized enzymes into a chimera efficiently couples the two reactions and reduces off-target proteolysis by almost sixfold. Hence, our modular approach may serve as a blueprint for engineering artificial nanofactories with reshaped catalytic performance and functionalities beyond those observed in natural systems. This study presents DNA-origami biocatalytic modular nanocompartments for programmed regulation of protein unfolding and degradation. These artificial nanofactories augment reaction kinetics, improve enzyme performance and reduce off-target effects.
在细胞内,化学反应通常通过模块化结构进行限制和组织。这有利于分子物种的定向定位及其高效转运到后续部位。在这里,我们介绍了一种无细胞纳米级模型,它利用区隔策略来进行受控蛋白质的展开和降解。我们的合成模型由两个相连的 DNA 折纸纳米小室组成(每个小室的尺寸为 25 nm × 41 nm × 53 nm):其中一个小室中装有蛋白质展开机 p97,另一个小室中装有蛋白酶糜蛋白酶。我们实现了 p97 在第一区室中的单向固定,建立了一个控制第二区室中底物招募、转运和加工的网关机制。我们的数据显示,虽然空间限制使单个反应的速率提高了 10 倍,但将隔室化的酶物理连接成嵌合体可有效地耦合两个反应,并将脱靶蛋白水解率降低近 6 倍。因此,我们的模块化方法可作为人工纳米工厂的工程蓝图,其催化性能和功能的重塑将超越自然系统。
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引用次数: 0
Exerting pulling forces in fluids by directional disassembly of microcrystalline fibres 通过定向分解微晶纤维在流体中施加拉力
IF 38.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-29 DOI: 10.1038/s41565-024-01742-x
L. C. Pantaleone, E. Calicchia, J. Martinelli, M. C. A. Stuart, Y. Y. Lopatina, W. R. Browne, G. Portale, K. M. Tych, T. Kudernac
Biomolecular polymerization motors are biochemical systems that use supramolecular (de-)polymerization to convert chemical potential into useful mechanical work. With the intent to explore new chemomechanical transduction strategies, here we show a synthetic molecular system that can generate forces via the controlled disassembly of self-organized molecules in a crystal lattice, as they are freely suspended in a fluid. An amphiphilic monomer self-assembles into rigid, high-aspect-ratio microcrystalline fibres. The assembly process is regulated by a coumarin-based pH switching motif. The microfibre crystal morphology determines the monomer reactivity at the interface, resulting in anisotropic etching. This effect exerts a directional pulling force on microscopic beads adsorbed on the crystal surface through weak multivalent interactions. We use optical-tweezers-based force spectroscopy to extract mechanistic insights into this process, quantifying a stall force of 2.3 pN (±0.1 pN) exerted by the ratcheting mechanism produced by the disassembly of the microfibres. Disassembling molecular microcrystalline fibres produce mechanical work by dragging micro objects along their surface via biased diffusion.
生物分子聚合马达是一种利用超分子(去)聚合作用将化学势转化为有用机械功的生物化学系统。为了探索新的化学机械传导策略,我们在这里展示了一种合成分子系统,当它们自由悬浮在流体中时,可以通过控制晶格中自组织分子的分解来产生力。一种两亲性单体可自组装成刚性、高纵横比的微晶纤维。组装过程由一种基于香豆素的 pH 值切换图案调节。微纤维晶体形态决定了界面上的单体反应性,从而导致各向异性蚀刻。这种效应通过微弱的多价相互作用,对吸附在晶体表面的微珠产生定向拉力。我们使用基于光学镊子的力谱仪来提取这一过程的机理,量化了微纤维解体产生的棘轮机制所产生的 2.3 pN(±0.1 pN)的滞留力。
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引用次数: 0
Embedding core–shell photovoltaic nanocells in organic optoelectronics 在有机光电子学中嵌入核壳光伏纳米电池
IF 38.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-29 DOI: 10.1038/s41565-024-01718-x
Tomoyuki Yokota, Yusaku Tagawa
Core–shell photovoltaic nanometre-scale cells are embedded in photo-crosslinkable organic semiconductors. This results in high performance and enables large-scale integration, thus overcoming the trade-off between photoelectric performance and device miniaturization.
纳米尺度的核壳光伏电池嵌入了光交联有机半导体。这不仅实现了高性能,而且实现了大规模集成,从而克服了光电性能与器件微型化之间的权衡。
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引用次数: 0
Silk fibroin as a surfactant for water-based nanofabrication 丝纤维素作为水基纳米制造的表面活性剂
IF 38.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-29 DOI: 10.1038/s41565-024-01720-3
Taehoon Kim, Beom Joon Kim, Giorgio E. Bonacchini, Nicholas A. Ostrovsky-Snider, Fiorenzo G. Omenetto
Water-based processing plays a crucial role in high technology, especially in electronics, material sciences and life sciences, with important implications in the development of high-quality reliable devices, fabrication efficiency, safety and sustainability. At the micro- and nanoscale, water is uniquely enabling as a bridge between biological and technological systems. However, new approaches are needed to overcome fundamental challenges that arise from the high surface tension of water, which hinders wetting and, thus, fabrication at the bio–nano interface. Here we report the use of silk fibroin as a surfactant to enable water-based processing of nanoscale devices. Even in minute quantities (for example, 0.01 w/v%), silk fibroin considerably enhances surface coverage and outperforms commercial surfactants in precisely controlling interfacial energy between water-based solutions and hydrophobic surfaces. This effect is ascribed to the amphiphilic nature of the silk molecule and its adaptive adsorption onto substrates with diverse surface energy, facilitating intermolecular interactions between unlikely pairs of materials. The approach’s versatility is highlighted by manufacturing water-processed nanodevices, ranging from transistors to photovoltaic cells. Its performance is found to be equivalent to analogous vacuum-processed devices, underscoring the utility and versatility of this approach for water-based nanofabrication. The amphiphilic nature of silk fibroin makes it a natural surfactant. Here it is shown to mediate interface interactions, enabling the wetting of hydrophobic surfaces with aqueous solutions and facilitating water-processed nanodevice fabrication without previous surface modification.
水基加工在高科技领域,尤其是电子学、材料科学和生命科学领域发挥着至关重要的作用,对开发高质量的可靠设备、提高制造效率、安全性和可持续性具有重要影响。在微米和纳米尺度上,水是连接生物和技术系统的独特桥梁。然而,水的高表面张力阻碍了生物纳米界面的润湿和制造,因此需要新的方法来克服由此带来的根本性挑战。在此,我们报告了使用丝纤维素作为表面活性剂来实现纳米级设备的水基加工。即使是微量(例如 0.01 w/v%),丝纤维素也能大大提高表面覆盖率,在精确控制水基溶液与疏水性表面之间的界面能方面优于商用表面活性剂。这种效果归因于蚕丝分子的两亲性及其对具有不同表面能的基质的适应性吸附,从而促进了不可能配对的材料之间的分子间相互作用。通过制造从晶体管到光伏电池的水处理纳米器件,凸显了这种方法的多功能性。其性能与类似的真空处理设备相当,突出了这种方法在水基纳米制造方面的实用性和多功能性。
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引用次数: 0
Charge-transfer contacts for the measurement of correlated states in high-mobility WSe2 用于测量高迁移率 WSe2 中相关态的电荷转移触点。
IF 38.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-25 DOI: 10.1038/s41565-024-01702-5
Jordan Pack, Yinjie Guo, Ziyu Liu, Bjarke S. Jessen, Luke Holtzman, Song Liu, Matthew Cothrine, Kenji Watanabe, Takashi Taniguchi, David G. Mandrus, Katayun Barmak, James Hone, Cory R. Dean
Two-dimensional semiconductors, such as transition metal dichalcogenides, have demonstrated tremendous promise for the development of highly tunable quantum devices. Realizing this potential requires low-resistance electrical contacts that perform well at low temperatures and low densities where quantum properties are relevant. Here we present a new device architecture for two-dimensional semiconductors that utilizes a charge-transfer layer to achieve large hole doping in the contact region, and implement this technique to measure the magnetotransport properties of high-purity monolayer WSe2. We measure a record-high hole mobility of 80,000 cm2 V–1 s–1 and access channel carrier densities as low as 1.6 × 1011 cm−2, an order of magnitude lower than previously achievable. Our ability to realize transparent contact to high-mobility devices at low density enables transport measurements of correlation-driven quantum phases including the observation of a low-temperature metal–insulator transition in a density and temperature regime where Wigner crystal formation is expected and the observation of the fractional quantum Hall effect under large magnetic fields. The charge-transfer contact scheme enables the discovery and manipulation of new quantum phenomena in two-dimensional semiconductors and their heterostructures. By utilizing the van der Waals electron acceptor α-RuCl3, this study establishes a p-type connection with WSe2, facilitating a high hole mobility of 80,000 cm2 V–1 s–1 for investigating quantum transport properties in a magnetic field of over 30 T.
二维半导体(如过渡金属二掺镓化合物)在开发高度可调的量子设备方面展现出巨大的潜力。要实现这一潜力,需要在低温和低密度条件下具有良好量子特性的低电阻电接触。在这里,我们介绍了一种利用电荷转移层实现接触区大空穴掺杂的二维半导体新器件结构,并利用这种技术测量了高纯度单层 WSe2 的磁传输特性。我们测得的空穴迁移率达到创纪录的 80,000 cm2 V-1 s-1,通道载流子密度低至 1.6 × 1011 cm-2,比以前可达到的水平低了一个数量级。我们能够在低密度条件下实现与高迁移率器件的透明接触,从而能够进行相关驱动量子相的传输测量,包括在预计会形成维格纳晶体的密度和温度条件下观察到低温金属-绝缘体转变,以及在大磁场条件下观察到分数量子霍尔效应。电荷转移接触方案有助于发现和操纵二维半导体及其异质结构中的新量子现象。
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引用次数: 0
A quantum sensor for atomic-scale electric and magnetic fields 原子尺度电场和磁场的量子传感器。
IF 38.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-25 DOI: 10.1038/s41565-024-01724-z
Taner Esat, Dmitriy Borodin, Jeongmin Oh, Andreas J. Heinrich, F. Stefan Tautz, Yujeong Bae, Ruslan Temirov
The detection of faint magnetic fields from single-electron and nuclear spins at the atomic scale is a long-standing challenge in physics. While current mobile quantum sensors achieve single-electron spin sensitivity, atomic spatial resolution remains elusive for existing techniques. Here we fabricate a single-molecule quantum sensor at the apex of the metallic tip of a scanning tunnelling microscope by attaching Fe atoms and a PTCDA (3,4,9,10-perylenetetracarboxylic-dianhydride) molecule to the tip apex. We address the molecular spin by electron spin resonance and achieve ~100 neV resolution in energy. In a proof-of-principle experiment, we measure the magnetic and electric dipole fields emanating from a single Fe atom and an Ag dimer on an Ag(111) surface with sub-angstrom spatial resolution. Our method enables atomic-scale quantum sensing experiments of electric and magnetic fields on conducting surfaces and may find applications in the sensing of spin-labelled biomolecules and of spin textures in quantum materials. The fabrication of a molecular quantum sensor on the tip of a scanning tunnelling microscope enables the detection of minute magnetic and electric fields of single atoms with sub-angstrom resolution.
在原子尺度上探测单电子自旋和核自旋产生的微弱磁场是物理学界长期面临的挑战。虽然目前的移动量子传感器实现了单电子自旋灵敏度,但原子空间分辨率仍然是现有技术难以实现的。在这里,我们通过将铁原子和 PTCDA(3,4,9,10-苝四羧酸二酐)分子附着在扫描隧穿显微镜金属尖端的顶点,制造出了单分子量子传感器。我们通过电子自旋共振来解决分子自旋问题,并实现了 ~100 neV 的能量分辨率。在原理验证实验中,我们以亚埃级的空间分辨率测量了 Ag(111) 表面上单个铁原子和 Ag 二聚体发出的磁场和电偶极子场。我们的方法实现了导电表面电场和磁场的原子尺度量子传感实验,可应用于自旋标记生物分子的传感和量子材料的自旋纹理。
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引用次数: 0
Competing light extraction strategies in perovskite light-emitting diodes 过氧化物发光二极管中相互竞争的光提取策略。
IF 38.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-25 DOI: 10.1038/s41565-024-01709-y
Guanding Mei, Kai Wang, Xiao Wei Sun
Light extraction is a key factor determining the efficiency of light-emitting diodes. This becomes more pronounced in high-refractive-index perovskite light-emitting diodes according to the ray-optics model. Photon recycling and microcavity effect are important ways to break through the ray-optics efficiency limit. However, these two effects are competing, that is, strategies to optimize them are mutually exclusive. For a breakthrough in efficiency, we should favour one of them and inhibit the other.
光提取是决定发光二极管效率的关键因素。根据射线光学模型,这在高折射率包晶发光二极管中变得更加明显。光子再循环和微腔效应是突破射线光学效率限制的重要途径。然而,这两种效应是相互竞争的,也就是说,优化这两种效应的策略是相互排斥的。要想在效率上有所突破,我们应该偏重其中一种效应,抑制另一种效应。
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引用次数: 0
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Nature nanotechnology
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