ACS Nano最新文献_第6页

On-Surface Synthesis and Cryogenic Exfoliation of Sterically Frustrated Atropisomers

IF 17.1 1区材料科学

ACS Nano Pub Date : 2025-04-01 DOI: 10.1021/acsnano.4c16645

Philipp D’Astolfo, J.G. Vilhena, Simon Rothenbühler, Carl Drechsel, Oscar Gutiérrez-Varela, Robert Häner, Silvio Decurtins, Shi-Xia Liu, Giacomo Prampolini, Rémy Pawlak, Ernst Meyer

{"title":"On-Surface Synthesis and Cryogenic Exfoliation of Sterically Frustrated Atropisomers","authors":"Philipp D’Astolfo, J.G. Vilhena, Simon Rothenbühler, Carl Drechsel, Oscar Gutiérrez-Varela, Robert Häner, Silvio Decurtins, Shi-Xia Liu, Giacomo Prampolini, Rémy Pawlak, Ernst Meyer","doi":"10.1021/acsnano.4c16645","DOIUrl":"https://doi.org/10.1021/acsnano.4c16645","url":null,"abstract":"On-surface synthesis provides exceptional control over nanostructure and material composition, enabling the creation of molecular compounds that are difficult or impossible to obtain with other synthesis methods. In this work, we demonstrate the possibility of synthesizing atropisomeric molecules made of chains of polyaromatic hydrocarbon units via on-surface synthesis. Scanning probe microscopy reveals that molecules adsorbed on Au(111) surfaces adopt a planar structure, with adjacent monomeric units aligning either in parallel or antiparallel configurations, influencing the alignment of the molecule on the surface. Cryo-force spectroscopy peeling experiments show that metastable conformers can be mechanically stabilized during the lifting-redeposition process of the polymer from the surface. In this process, periodic drops in frequency shift are observed, corresponding to monomer detachment-readsorption. Interestingly, this periodicity is independent of the parallel/antiparallel configuration but is counterintuitively smaller than the monomer size. Molecular dynamics simulations relate this effective reduction in unit length to a tethering effect between the chain and the surface. This, in turn, allowed us to test and validate Silva’s analytical phenomenological power law model for peeling. Our findings not only provide a method for studying the elusive class 1 atropisomeric molecules but also offer deeper insight into the peeling phenomenon at the nanoscale.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"388 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758624","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

Transient Macrophage Depletion Circumvents Scavenging and Redirects Biodistribution of mRNA-Lipid Nanoparticles

IF 17.1 1区材料科学

ACS Nano Pub Date : 2025-04-01 DOI: 10.1021/acsnano.5c02001

Zhefan Yuan, Sijin Luozhong, Ruoxin Li, Wenchao Gu, Yu Chen, Dani Bhashyam, Rachel Lai, Shaoyi Jiang

{"title":"Transient Macrophage Depletion Circumvents Scavenging and Redirects Biodistribution of mRNA-Lipid Nanoparticles","authors":"Zhefan Yuan, Sijin Luozhong, Ruoxin Li, Wenchao Gu, Yu Chen, Dani Bhashyam, Rachel Lai, Shaoyi Jiang","doi":"10.1021/acsnano.5c02001","DOIUrl":"https://doi.org/10.1021/acsnano.5c02001","url":null,"abstract":"The mononuclear phagocytic system is recognized as a major scavenger of mRNA-lipid nanoparticles (LNPs), clearing and redirecting these particles away from their intended targets and thus diminishing their delivery efficacy. Understanding the mechanism by which mRNA-LNPs interact with phagocytes and how this interaction affects the mRNA transfection is critical to enhancing the delivery of mRNA. In this study, we temporarily depleted both circulating and resident macrophages (MF) and evaluated the transfection efficiency and biodistribution of mRNA-LNPs. We first demonstrated the enhanced liver expression using two liver-tropic formulations and the significant improvement of the in vivo gene editing efficiency of CRISPR-Cas9 in the Ai14 mouse model after MF depletion, providing a versatile strategy for enhanced mRNA delivery to the liver regardless of the formulation employed. We then extended our investigations to lung-tropic and lymphoid-tropic LNP formulations and discovered that MF depletion abolishes the targeting capacities of these non-liver-tropic formulations, providing insights into the organ targeting of LNPs. Finally, we screened and compared various clinically relevant MF depletion methods, providing the translation potential of this method on enhanced hepatic delivery of mRNA.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"55 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745236","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

Carboxysome Shell Protein CcmK2 Assembles into Monodisperse and pH-Reversible Microparticles

IF 17.1 1区材料科学

ACS Nano Pub Date : 2025-03-31 DOI: 10.1021/acsnano.4c18021

Claudia A. Mak, Vincent Chriscoli, Vinson Lam, Jing Yang, Lu-Ning Liu, Anthony G. Vecchiarelli

{"title":"Carboxysome Shell Protein CcmK2 Assembles into Monodisperse and pH-Reversible Microparticles","authors":"Claudia A. Mak, Vincent Chriscoli, Vinson Lam, Jing Yang, Lu-Ning Liu, Anthony G. Vecchiarelli","doi":"10.1021/acsnano.4c18021","DOIUrl":"https://doi.org/10.1021/acsnano.4c18021","url":null,"abstract":"Synthetic nano- and microparticles have become essential tools in biotechnology. Protein-based compartments offer distinct advantages over synthetic particles, such as biodegradability and biocompatibility, but their development is still in its infancy. Bacterial microcompartments (BMCs) are protein-based organelles consisting of a protein shell encapsulating an enzymatic core. BMCs are self-assembling, selectively permeable, and modular, making them ideal candidates for the development of protein compartments for biotechnology. Indeed, several groups have engineered BMC shells and individual shell proteins into synthetic nanoreactors and functionalized molecular scaffolds. Expanding the variety of architectures assembled from BMC shell proteins will increase their versatility as building blocks in biotechnology. Here, we developed a method for the in vitro assembly of single-component monodisperse microparticles using only CcmK2, the major hexameric shell protein of the β-carboxysome BMC. We report the controlled assembly of a single type of BMC shell protein into a solid microparticle. High-resolution imaging revealed CcmK2 particles to be assemblies of radially clustered nanotubes. Through biochemical characterization, we determined the conditions for reversible assembly and residues mediating assembly. We found that pH is a key regulator of final particle size and disassembly. Our study situates CcmK2 particles as precisely controlled and self-assembling monodisperse solid protein particles for future applications in biotechnology.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"25 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745261","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

In Situ H2S-Releasing Stents Optimize Vascular Healing

IF 17.1 1区材料科学

ACS Nano Pub Date : 2025-03-31 DOI: 10.1021/acsnano.4c16345

Jiayi Zhang, Yang Li, Zhen Xiang, Hongxia Pu, Cheng Ji, Xingrong Ren, Daihua Fu, Yunbing Wang

{"title":"In Situ H2S-Releasing Stents Optimize Vascular Healing","authors":"Jiayi Zhang, Yang Li, Zhen Xiang, Hongxia Pu, Cheng Ji, Xingrong Ren, Daihua Fu, Yunbing Wang","doi":"10.1021/acsnano.4c16345","DOIUrl":"https://doi.org/10.1021/acsnano.4c16345","url":null,"abstract":"Stent implantation remains a cornerstone of interventional cardiology, providing a minimally invasive solution to restore blood flow in occluded vessels. However, current stents face persistent challenges in simultaneously preventing neointimal hyperplasia and promoting reendothelialization, compromising their long-term efficacy. To address these limitations, we developed an in situ H2S-releasing polymer brush-coated stent that actively modulates material–blood interactions, creating a favorable microenvironment for vascular healing. H2S enhances the stent’s antithrombotic properties by inhibiting fibrinogen binding and platelet activation, while also mitigating oxidative stress and promoting macrophage polarization toward the anti-inflammatory M2 phenotype. In vivo, the H2S-releasing stents significantly improved vascular healing by accelerating endothelialization and inhibiting smooth muscle cell overproliferation, resulting in a thinner neointima with functional endothelial coverage. Transcriptomic analysis further elucidated the underlying mechanisms, revealing H2S-mediated modulation of key biological pathways that support vascular healing. These findings underscore the potential of in situ H2S release as an effective strategy for optimizing vascular implants and improving long-term outcomes.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"45 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736927","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

Regulating the Tumor Microbiome through Near-Infrared-III Light-Excited Photosynthesis

IF 17.1 1区材料科学

ACS Nano Pub Date : 2025-03-31 DOI: 10.1021/acsnano.4c18954

Feiyu Li, Bingzhu Zheng, Jiafei Chen, Qilong Yan, Zijie Lu, Chao Fang, Yike Fu, Xiang Li

引用次数: 0

Nonlinear Optical Resonances from Ballistic Electron Funnelling.

IF 15.8 1区材料科学

ACS Nano Pub Date : 2025-03-31 DOI: 10.1021/acsnano.5c00169

Hue T B Do, Gregory K Ngirmang, Lin Wu, Michel Bosman

引用次数: 0

Controlled Sensing of User-Defined Aptamer-Based Targets Using Scanning Ionic Conductance Spectroscopy.

IF 15.8 1区材料科学

ACS Nano Pub Date : 2025-03-31 DOI: 10.1021/acsnano.4c18509

Helena Miljkovic, Lely Feletti, Gordanna Pistoletti Blanchet, Marcos Penedo, Zahra Ayar, Barney Drake, Alexandre Kuhn, Wayne Yang, Georg E Fantner, Aleksandra Radenovic

{"title":"Controlled Sensing of User-Defined Aptamer-Based Targets Using Scanning Ionic Conductance Spectroscopy.","authors":"Helena Miljkovic, Lely Feletti, Gordanna Pistoletti Blanchet, Marcos Penedo, Zahra Ayar, Barney Drake, Alexandre Kuhn, Wayne Yang, Georg E Fantner, Aleksandra Radenovic","doi":"10.1021/acsnano.4c18509","DOIUrl":"https://doi.org/10.1021/acsnano.4c18509","url":null,"abstract":"Solid-state nanopores offer the possibility of detecting disease biomarkers in early diagnostic applications. Standard approaches harness fingerprinting, where protein targets are bound to DNA carriers and detected in free translocation with a solid-state nanopore. However, they suffer from several drawbacks, including uncontrolled fast translocations, which lead to low detection accuracy and a low signal-to-noise ratio (SNR). This has hampered their application in clinical settings. Here, we propose a nanopore-based system capable of sensing selected molecules of interest from biological fluids by harnessing programmable aptamer sequences attached to DNA carrier systems that are tethered to glass surfaces. This allows for spatial and velocity control over translocation in the x, y, and z directions and enables the repeated scanning of the same analyte. The scanning ion conductance spectroscopy (SICS) based approach distinguishes itself from standard nanopore-based approaches with its ability to repeatedly scan the same aptamer molecule target site more than 5 times. We designed a DNA carrier with multiple binding sites for different aptamers to increase the yield of the experiment. Our approach achieves a detection rate of up to 74%, significantly higher than the 14% achieved with standard solid-state nanopore measurements. The strong spatial control also allows for significantly increased densities of aptamer target sites along the same DNA carrier, thereby paving the way for multiplexed sensing. The system offers user-defined programmability with different aptamer sequences, potentially expanding the use of our system to sense other disease biomarkers.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":" ","pages":""},"PeriodicalIF":15.8,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143750252","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

Field-Free Spin–Orbit Torque Switching of Canted van der Waals Magnets

IF 17.1 1区材料科学

ACS Nano Pub Date : 2025-03-31 DOI: 10.1021/acsnano.4c16826

Bing Zhao, Lalit Pandey, Khadiza Ali, Erdi Wang, Craig M. Polley, Balasubramanian Thiagarajan, Peter Makk, Marcos H. D. Guimarães, Saroj Prasad Dash

{"title":"Field-Free Spin–Orbit Torque Switching of Canted van der Waals Magnets","authors":"Bing Zhao, Lalit Pandey, Khadiza Ali, Erdi Wang, Craig M. Polley, Balasubramanian Thiagarajan, Peter Makk, Marcos H. D. Guimarães, Saroj Prasad Dash","doi":"10.1021/acsnano.4c16826","DOIUrl":"https://doi.org/10.1021/acsnano.4c16826","url":null,"abstract":"Spin–orbit torque (SOT) magnetization switching is crucial for next-generation energy-efficient spintronic technologies. The recent discovery of van der Waals (vdW) magnets holds promise for such SOT phenomena because of their tunable magnetic properties. However, a demonstration of energy-efficient and field-free SOT switching of vdW magnets is required for their potential applications. Here, we demonstrate field-free and deterministic switching using an intrinsic canted vdW magnet Fe5GeTe2 in a heterostructure with Pt having a larger spin Hall conductivity up to room temperature. Using anomalous Hall electrical detection for magnetization readout, we reveal that field-free deterministic SOT switching in the Fe5GeTe2/Pt Hall devices can be attributed to the canted magnetic anisotropy of Fe5GeTe2, originating from its crystal and magnetic structures. Detailed second harmonic Hall measurements exhibit a high spin Hall conductivity σSH ∼ 3 × 105ℏ/2e Ω–1m–1 with an SOT effective damping-like field of 0.06 mT per MA/cm2. These findings reveal efficient and field-free SOT phenomena in the canted vdW magnet Fe5GeTe2 up to room temperature and highlight their usefulness in spintronic devices.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"103 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736929","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

Nanocomposite Hydrogels and Micro/Nanostructures for Printing Organoids.

IF 15.8 1区材料科学

ACS Nano Pub Date : 2025-03-31 DOI: 10.1021/acsnano.4c17587

Daixi Xie, Bingda Chen, Wenqing Wang, Wenjing Guo, Zhiyuan Sun, Long Wang, Bin Shi, Yanlin Song, Meng Su

引用次数: 0

Reactive Molecular Beam Epitaxy Growth of a 1T-FeS₂ Single-Layer-Atomic Structure, Moiré, and Decoupling via Intercalation.

IF 15.8 1区材料科学

ACS Nano Pub Date : 2025-03-31 DOI: 10.1021/acsnano.4c17873

Mahesh Krishna Prabhu, Philippe David, Valérie Guisset, Lucio Martinelli, Johann Coraux, Gilles Renaud

{"title":"Reactive Molecular Beam Epitaxy Growth of a 1T-FeS2 Single-Layer-Atomic Structure, Moiré, and Decoupling via Intercalation.","authors":"Mahesh Krishna Prabhu, Philippe David, Valérie Guisset, Lucio Martinelli, Johann Coraux, Gilles Renaud","doi":"10.1021/acsnano.4c17873","DOIUrl":"https://doi.org/10.1021/acsnano.4c17873","url":null,"abstract":"Two-dimensional (2D) iron disulfide (FeS2), in its 1T polymorph, is a promising candidate for high-Curie-temperature ferromagnetic applications. Unlike typical van der Waals materials, FeS2 lacks a naturally lamellar bulk structure and thus cannot be prepared by exfoliation. Consequently, it exists solely as a synthetic 2D magnet, primarily produced via chemical vapor deposition. Here, we propose an alternative synthesis method: reactive molecular beam epitaxy, where an iron layer predeposited on a Au(111) substrate is sulfurized to form FeS2. Structural and compositional analyses of the resulting 2D layer─employing scanning tunneling microscopy, electron diffraction, Auger electron spectroscopy, and synchrotron surface X-ray diffraction─confirm a nominal Fe ratio of 1:2, essential for achieving a high Curie temperature. Modeling and fitting the three-dimensional X-ray diffraction data further reveals that the layer crystallizes in the desired 1T polymorph. This 1T-FeS2 grown on Au(111) exhibits exceptional crystalline quality, largely surpassing that of other 2D transition metal dichalcogenides epitaxially grown on substrates. In addition, it shows pronounced atomic distortions from an ideal 1T structure, attributed to the strain induced by the substrate to achieve a perfectly commensurate 5 × 5 moiré pattern. The 1T-FeS2 and moiré atomic structures are fully determined with high accuracy on atomic coordinates. Finally, through Cs intercalation, we demonstrate complete decoupling of the FeS2 layer from the substrate and the release of heteroepitaxial strains.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":" ","pages":""},"PeriodicalIF":15.8,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143750256","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