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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
Oral administration of garlic-derived nanoparticles improves cancer immunotherapy by inducing intestinal IFNγ-producing γδ T cells 口服大蒜衍生纳米颗粒可通过诱导肠道IFNγ产生γδT细胞改善癌症免疫疗法。
IF 38.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-25 DOI: 10.1038/s41565-024-01722-1
Jialu Xu, Yue Yu, Yue Zhang, Huaxing Dai, Qianyu Yang, Beilei Wang, Qingle Ma, Yitong Chen, Fang Xu, Xiaolin Shi, Zhuang Liu, Chao Wang
Gamma-delta (γδ) T cell-based cancer immunotherapies represent a promising avenue for cancer treatment. However, their development is challenged by the limited expansion and differentiation of the cells ex vivo. Here we induced the endogenous expansion and activation of γδ T cells through oral administration of garlic-derived nanoparticles (GNPs). We found that GNPs could significantly promote the proliferation and activation of endogenous γδ T cells in the intestine, leading to generation of large amount of interferon-γ (IFNγ). Moreover GNP-treated mice showed increased levels of chemokine CXCR3 in intestinal γδ T cells, which can drive their migration from the gut to the tumour environment. The translocation of γδ T cells and IFNγ from the intestine to extraintestinal subcutaneous tumours remodels the tumour immune microenvironment and synergizes with anti-PD-L1, inducing robust antitumour immunity. Our study delineates mechanistic insight into the complex gut–tumour interactome and provides an alternative approach for γδ T cell-based immunotherapy. γδ T cell-based immunotherapies are limited by the reduced expansion and activation of the T cells ex vivo. Here the authors show that garlic nanoparticles can activate IFNγ-producing γδ T cells directly in the intestine, before they translocate to extraintestinal tumours, where they can synergize with anti-PD-L1 therapy, inducing robust antitumour immunity.
以γ-δ(γδ)T 细胞为基础的癌症免疫疗法是一种前景广阔的癌症治疗方法。然而,由于这些细胞在体内的扩增和分化有限,它们的发展面临挑战。在这里,我们通过口服大蒜提取的纳米颗粒(GNPs)诱导了γδT细胞的内源性扩增和活化。我们发现,GNPs 能显著促进肠道内源性 γδ T 细胞的增殖和活化,从而产生大量干扰素-γ(IFNγ)。此外,经 GNP 处理的小鼠肠道γδ T 细胞中趋化因子 CXCR3 水平升高,这可促使它们从肠道迁移到肿瘤环境中。γδT细胞和IFNγ从肠道转移到肠道外的皮下肿瘤会重塑肿瘤免疫微环境,并与抗PD-L1协同作用,诱导强大的抗肿瘤免疫。我们的研究从机理上揭示了复杂的肠道-肿瘤相互作用组,为基于γδT细胞的免疫疗法提供了另一种方法。
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引用次数: 0
Breaking barriers by interfacial charge transfer 通过界面电荷转移打破障碍
IF 38.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-25 DOI: 10.1038/s41565-024-01703-4
Youngwook Kim
The issue of ohmic contact in WSe2 has been effectively addressed through a significant charge transfer mechanism enabled by the RuCl3/WSe2 heterostructure.
通过 RuCl3/WSe2 异质结构促成的重要电荷转移机制,WSe2 中的欧姆接触问题得到了有效解决。
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引用次数: 0
Deterministic switching of perpendicular magnetization by out-of-plane anti-damping magnon torques 通过平面外反阻尼磁子转矩实现垂直磁化的确定性切换。
IF 38.1 1区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2024-07-24 DOI: 10.1038/s41565-024-01741-y
Fei Wang, Guoyi Shi, Dongsheng Yang, Hui Ru Tan, Chenhui Zhang, Jiayu Lei, Yuchen Pu, Shuhan Yang, Anjan Soumyanarayanan, Mehrdad Elyasi, Hyunsoo Yang
Spin-wave excitations of magnetic moments (or magnons) can transport spin angular momentum in insulating magnetic materials. This property distinguishes magnonic devices from traditional electronics, where power consumption results from electrons’ movement. Recently, magnon torques have been used to switch perpendicular magnetization in the presence of an external magnetic field. Here we present a material system composed of WTe2/antiferromagnetic insulator NiO/ferromagnet CoFeB heterostructures that allows magnetic field-free switching of the perpendicular magnetization. The magnon currents, with a spin polarization canting of −8.5° relative to the sample plane, traverse the 25-nm-thick polycrystalline NiO layer while preserving their original polarization direction, subsequently exerting an out-of-plane anti-damping magnon torque on the ferromagnetic layer. Using this mechanism, we achieve a 190-fold reduction in power consumption in PtTe2/WTe2/NiO/CoFeB heterostructures compared to Bi2Te3/NiO/CoFeB control samples, which only exhibit in-plane magnon torques. Our field-free demonstration contributes to the realization of all-electric, low-power, perpendicular magnetization switching devices. Control of magnetization is at the core of many spintronic applications. Out-of-plane anti-damping magnon torque now enables low-power, deterministic switching of perpendicular magnetization at zero magnetic field.
磁矩(或磁子)的自旋波激发可在绝缘磁性材料中传输自旋角动量。这一特性使磁子设备有别于传统的电子设备,后者的功耗来自电子运动。最近,磁子力矩已被用于在外部磁场存在的情况下切换垂直磁化。在这里,我们介绍了一种由 WTe2/反铁磁绝缘体 NiO/铁磁体 CoFeB 异质结构组成的材料系统,它可以实现垂直磁化的无磁场切换。磁子电流相对于样品平面的自旋极化倾斜度为-8.5°,在保持其原始极化方向的同时穿过 25 纳米厚的多晶氧化镍层,随后在铁磁层上施加平面外抗阻尼磁子力矩。利用这种机制,我们实现了 PtTe2/WTe2/NiO/CoFeB 异质结构的功耗比 Bi2Te3/NiO/CoFeB 对照样品降低 190 倍,而 Bi2Te3/NiO/CoFeB 对照样品只表现出平面内的磁子力矩。我们的无磁场演示有助于实现全电、低功耗、垂直磁化开关器件。
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引用次数: 0
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Nature nanotechnology
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