ACS Nano最新文献

{"title":"Charge Transfer of Metal Porphyrins on a NaCl Thin Film Observed by Scanning Tunneling Microscopy in the Transport Gap.","authors":"Li-Qing Zheng,Abhishek Grewal,Kelvin Anggara,Fábio J R Costa,Christopher C Leon,Klaus Kuhnke,Klaus Kern","doi":"10.1021/acsnano.5c01235","DOIUrl":"https://doi.org/10.1021/acsnano.5c01235","url":null,"abstract":"Elucidating the electronic structure of organic molecules in contact with a dielectric layer is essential to understanding and controlling many important processes, such as catalysis, photochemistry, and electroluminescence. However, this challenge calls for a detailed characterization of molecule-dielectric contacts on the atomic scale. Here, we employ scanning tunneling microscopy (STM) at low temperature (4 K) in combination with ab initio calculations to investigate the subnanometer-scale electronic states of photoactive molecules on a dielectric surface. For platinum and palladium octaethylporphyrin (PtOEP and PdOEP) adsorbed on few layers of NaCl on a metal substrate, our STM imaging of them in the energy gap between the frontier orbitals demonstrates their high sensitivity to the local environment, namely, adsorption site and applied voltage. Our calculations reveal that the states in this energy gap originate from combinations of molecular orbitals far from the Fermi level and that they are affected by the extent of molecule-surface partial charge transfer, which is tuned by adsorption site and voltage in the tunnel junction.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"47 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143915221","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}

{"title":"Multivalent Aptamer Assembly Enhances Tumor-Specific Degradation of Transforming Growth Factor-Beta to Remodel the Stromal and Immunosuppressive Cancer Microenvironment","authors":"Yan Liu, Xinyue Ran, Guangdong Zhou, Yingbin Liu, Weihong Tan","doi":"10.1021/acsnano.4c16628","DOIUrl":"https://doi.org/10.1021/acsnano.4c16628","url":null,"abstract":"Extracellular proteins like transforming growth factor-β (TGFβ) are crucial enforcers in the development of cancer stroma and the tumor immunosuppressive microenvironment. Lysosome-targeting chimera-mediated protein degradation appeared as a promising tool for extracellular signal interference but was limited by several lysosome-trafficking receptors and inadequate in vivo degradation efficiency. Here, we designed a multivalent aptamer assembly with a universal pattern to drag extracellular proteins (e.g., TGFβ1) for lysosome degradation with high tumor specificity. By accelerating cell recognition-internalization and lysosomal delivery, the assembly promoted TGFβ blockade and degradation in pancreatic cancer cells and pancreatic stellate cells (PSCs). In vivo, the assembly exhibited highly tumor-specific accumulation and prolonged retention, which resulted in efficient TGFβ inhibition, stromal remodeling, and reversed polarization of immunosuppressive cells in the tumor microenvironment, as well as synergic therapeutic effects when combined with gemcitabine or ovalbumin. Therefore, this study provides a feasible strategy to construct a multivalent aptamer assembly for tumor-specific extracellular protein degradation, after remodeling the tumor stromal and immunosuppressive microenvironment in a manner that enhances the effects of cancer chemotherapy and immunotherapy.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"19 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143910728","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}

{"title":"Identifying In Situ Activity and Selectivity of Oxygen Reduction Catalysts at the Subparticle Level","authors":"Yufei Yao, Hongyang Qu, Zehui Sun, Yequan Chen, Shenglong Yang, Wei Ma","doi":"10.1021/acsnano.5c01902","DOIUrl":"https://doi.org/10.1021/acsnano.5c01902","url":null,"abstract":"Oxygen reduction reaction (ORR) plays a crucial role in both the chemical and energy industries. Despite substantial advancements in theoretical, computational, and experimental studies, identifying both the in situ activity and selectivity in ORR electrocatalysis remains a major challenge. Here, using a suite of correlative operando scanning electrochemical probe and electrochemiluminescence microscopy techniques, we establish a link between the morphological structure and the local ORR activity and selectivity of single Au and Au@Pt platelets at the subparticle level. It is clearly shown that the edge facets of Au and Au@Pt platelets exhibit higher activity for 4e^– ORR compared to basal planes, whereas the basal planes of both Au and Au@Pt platelets demonstrate superior 2e^– selectivity relative to the edge facets. These findings deepen our understanding of ORR activity and selectivity across different facets at the subparticle level, which offers valuable guidance for the rational design of highly efficient ORR electrocatalysts.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"116 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143915930","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}

{"title":"Reproducible Transpalpebral Intraocular Pressure Sensing Enabled by Low-Energy-Barrier Ion Pumping","authors":"Xueyang Ren, Xuefei Zhu, Xiaodong Shao, Wen Yang, Yanmei Meng, Shiyu Chen, Yannan Wang, Jianqing Li, Qin Jiang, Benhui Hu","doi":"10.1021/acsnano.5c02762","DOIUrl":"https://doi.org/10.1021/acsnano.5c02762","url":null,"abstract":"Elevated intraocular pressure (IOP) is a major risk factor for blindness in glaucoma patients, highlighting the critical need for continuous IOP monitoring. While traditional transpalpebral tonometers (TTs) circumvent corneal contact by adopting Goldmann applanation principles through impulsive corneal flattening forces, their measurement accuracy is inherently compromised by eyelid-induced cushion effects. In contrast, parallel-plate capacitive sensors employ constant compressive loading upon the eyelid, achieving palpebral compaction to mitigate the cushion effects. More recently, ion-pump-based capacitive sensors have emerged as promising alternatives, particularly due to their enhanced sensitivity. Nevertheless, these sensors exhibit sharp sensitivity deterioration at extended measurement ranges (0–10 kPa). This operational constraint originates from the strong hydrogen bond energies (between confining matrices and ions) and rigid block copolymer matrices’ steric hindrance. To address these limitations, we developed a transpalpebral tonometer featuring low-energy-barrier ion pumps, incorporating (3-aminopropyl)triethoxysilane (APTES)-silanized liquid metal nanoparticles (LM NPs) as confining matrices and an ionic liquid as an ion donor. The low-energy barrier arises from (1) weaker hydrogen bonds between the N–H of APTES and the F of the ionic liquid and (2) reduced crystallinity in the elastomeric matrices induced by LM NPs. Our sensor achieves a sensitivity of 24.88 kPa^–1 with maintained linearity over 0–85 kPa. In vivo animal trials over 120 min validated its continuous IOP monitoring capability, reliably detecting elevated IOP states and demonstrating clinical potential for glaucoma management.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"74 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143910780","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}

{"title":"Strain-Induced Charge Density Waves with Emergent Topological States in Monolayer NbSe2","authors":"Wei-Chi Chiu, Sougata Mardanya, Robert Markiewicz, Jouko Nieminen, Bahadur Singh, Tugrul Hakioglu, Amit Agarwal, Tay-Rong Chang, Hsin Lin, Arun Bansil","doi":"10.1021/acsnano.4c13478","DOIUrl":"https://doi.org/10.1021/acsnano.4c13478","url":null,"abstract":"Emergence of topological states in strongly correlated systems, particularly two-dimensional (2D) transition-metal dichalcogenides, offers a platform for manipulating electronic properties in quantum materials. However, a comprehensive understanding of the intricate interplay between correlations and topology remains elusive. Here we employ first-principles modeling to reveal two distinct 2 × 2 charge density wave (CDW) phases in monolayer 1H-NbSe<sub>2</sub>, which become energetically favorable over the conventional 3 × 3 CDWs under modest biaxial tensile strain of about 1%. These strain-induced CDW phases coexist with numerous topological states characterized by <i></i><span style=\"color: inherit;\"></span><span data-mathml='<math xmlns=\"http://www.w3.org/1998/Math/MathML\" display=\"inline\"><msub><mrow><mi mathvariant=\"double-struck\">Z</mi></mrow><mrow><mn>2</mn></mrow></msub></math>' role=\"presentation\" style=\"position: relative;\" tabindex=\"0\"><nobr aria-hidden=\"true\"><span style=\"width: 1.253em; display: inline-block;\"><span style=\"display: inline-block; position: relative; width: 1.139em; height: 0px; font-size: 110%;\"><span style=\"position: absolute; clip: rect(1.31em, 1001.14em, 2.503em, -999.997em); top: -2.156em; left: 0em;\"><span><span><span style=\"display: inline-block; position: relative; width: 1.139em; height: 0px;\"><span style=\"position: absolute; clip: rect(3.128em, 1000.68em, 4.151em, -999.997em); top: -3.974em; left: 0em;\"><span><span style=\"font-family: STIXMathJax_DoubleStruck;\">ℤ</span></span><span style=\"display: inline-block; width: 0px; height: 3.98em;\"></span></span><span style=\"position: absolute; top: -3.804em; left: 0.741em;\"><span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Main;\">2</span></span><span style=\"display: inline-block; width: 0px; height: 3.98em;\"></span></span></span></span></span><span style=\"display: inline-block; width: 0px; height: 2.162em;\"></span></span></span><span style=\"display: inline-block; overflow: hidden; vertical-align: -0.247em; border-left: 0px solid; width: 0px; height: 1.003em;\"></span></span></nobr><span role=\"presentation\"><math display=\"inline\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><msub><mrow><mi mathvariant=\"double-struck\">Z</mi></mrow><mrow><mn>2</mn></mrow></msub></math></span></span><script type=\"math/mml\"><math display=\"inline\"><msub><mrow><mi mathvariant=\"double-struck\">Z</mi></mrow><mrow><mn>2</mn></mrow></msub></math></script> topology, high mirror Chern numbers, topological nodal lines, and higher-order topological states, which we have verified rigorously by computing the topological indices and the presence of robust edge states and localized corner states. Remarkably, these topological properties emerge because of the CDW rather than a pre-existing topology in the pristine phase. These results elucidate the interplay between correlations, topology, and geometry in 2D materials and ind","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"9 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143915932","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}

{"title":"Multiphoton-Excited Upconversion Luminescence and Amplified Spontaneous Emission from Te4+-Doped Cs2SnCl6 Nanocrystals","authors":"Wei Zhang, Wei Zheng, Lingyun Li, Xiaoying Shang, Ping Huang, Xiaodong Yi, Hao Zhang, Yan Yu, Xueyuan Chen","doi":"10.1021/acsnano.5c05992","DOIUrl":"https://doi.org/10.1021/acsnano.5c05992","url":null,"abstract":"High-order nonlinear multiphoton absorption (MPA) is technologically important for a variety of photonic and biological applications owing to its superior advantages over linear absorption and low-order MPA such as greater spatial confinement, larger penetration depth, reduced autofluorescence, and enhanced imaging resolution. However, practical implementation beyond three-photon processes remains notoriously difficult due to the sharp reduction of absorption cross sections with increasing nonlinearity and inherent material instability under high-density irradiation. Herein, we address these challenges through rationally designed Te⁴⁺-doped Cs₂SnCl₆ nanocrystals (NCs), which demonstrate wideband nonlinear responsiveness across 800–2600 nm, allowing achievement of two- to seven-photon absorption (PA) with cross sections outperforming conventional nonlinear optical materials. Particularly, the engineered NCs enable 3PA-excited amplified spontaneous emission (ASE) with an ultralow excitation threshold of 0.22 μJ cm^–2 under a 1300 nm femtosecond-pulsed laser excitation, representing 1–4 orders of magnitude improvement compared to existing nonlinear ASE systems. This work presents the excellent 7PA properties in metal halide NCs, positioning lead-free metal halide NCs promising as efficient light-emitting materials for extreme nonlinear nanophotonics.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"11 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143910781","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}

{"title":"Unveiling Mechanically Driven Catalytic Processes: Beyond Piezocatalysis to Synergetic Effects","authors":"Yue Jiang, Jun Liang, Fenglin Zhuo, Hongyang Ma, Sajjad S. Mofarah, Charles C. Sorrell, Danyang Wang, Pramod Koshy","doi":"10.1021/acsnano.5c02660","DOIUrl":"https://doi.org/10.1021/acsnano.5c02660","url":null,"abstract":"Mechanically driven catalysis (MDC) has emerged as an effective strategy for environmental remediation, renewable energy conversion, and cancer therapy; this functions by converting mechanical forces to drive catalytic reactions. This review examines four primary mechanisms, namely, piezocatalysis, flexocatalysis, tribocatalysis, and sonocatalysis, each involving specific catalytic pathways for harnessing mechanical energy at the nanoscale. However, significant challenges arise in decoupling the effects related to each individual mechanism in order to better understand and manipulate their synergies. In this review, the fundamental principles underpinning MDC are systematically interpreted. Beyond mechanistic insights, recent advancements in performance enhancement strategies for these catalysts are highlighted. Potential applications using these mechanistic approaches in environmental remediation (pollutant and antibiotic degradation and microbial disinfection), renewable energy conversion (hydrogen production and greenhouse gas conversion), and biomedical treatments (particularly cancer therapy) are discussed. Finally, the mechanistic synergies and limiting factors are explored, addressing challenges related to the overlooked combined effects of ultrasound as the activation source, complexities in mechanical force interactions at the nanoscale, and the need for targeted application strategies. Additionally, the industrial potential of these catalytic processes with consideration to scalability and practical deployment is evaluated. While challenges remain, this review provides a roadmap for advancing mechanically driven catalyst design and implementation toward real-world applications, offering potential into its future trajectory and transformative impact across numerous fields.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"47 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143915771","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}

{"title":"Quantum and Classical Exceptional Points at the Nanoscale: Properties and Applications","authors":"Yu-Wei Lu, Wei Li, Xue-Hua Wang","doi":"10.1021/acsnano.4c15648","DOIUrl":"https://doi.org/10.1021/acsnano.4c15648","url":null,"abstract":"Exceptional points (EPs) are the spectral singularities and one of the central concepts of non-Hermitian physics, originating from the inevitable energy exchange with the surrounding environment. EPs exist in diverse physical systems and give rise to many counterintuitive effects, offering rich opportunities to control the dynamics and alter the properties of optical, electronic, acoustic, and mechanical states. The last two decades have witnessed the flourishing of non-Hermitian physics and associated applications related to coalesced eigenstates at EPs in a plethora of classical systems. While stemming from the quantum mechanism, the implementation of EPs in real quantum systems still faces challenges of tuning and stabilizing the systems at EPs, as well as the additional noises that hinder the observation of relevant phenomena. This review mainly focuses on summarizing the current efforts and opportunities offered by quantum EPs that result from or produce observable quantum effects. We introduce the concepts of Hamiltonian and Liouvillian EPs in the quantum regime and focus on their different properties in connection with quantum jumps and decoherence. We then provide a comprehensive discussion covering the theoretical and experimental advances in accessing EPs in diverse quantum systems and platforms. Special attention is paid to EP-based quantum-optics applications with state-of-art technologies. Finally, we present a discussion on the existing challenges of constructing quantum EPs at the nanoscale and an outlook on the fundamental science and applied technologies of quantum EPs, aiming to provide valuable insights for future research and building quantum devices with high performance and advanced functionalities.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"3 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143910777","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}

{"title":"Ultrastiff Bioinspired Protein–Carbon Nanotube Hybrid Sponge with Shape Memory Effects","authors":"Yang Yang, Yingjie Cao, Shengjie Li, Yana Wang, Xiaohua Zhang, Yitan Li, Zhaohui Yang","doi":"10.1021/acsnano.5c06297","DOIUrl":"https://doi.org/10.1021/acsnano.5c06297","url":null,"abstract":"Natural protein-based biomaterials with complex hierarchical structures often have incredible and even counterintuitive mechanical properties. Understanding and utilizing the conformational transition mechanisms of natural proteins will further guide the design of natural-inspired biomaterials. In this study, a small static-force-induced spatiotemporal “freezing” phenomenon of silk fibroins confined in porous carbon nanotube sponges has been investigated. The “freezing” silk fibroins not only bring the shape memory effect to elastic carbon nanotube sponges but also enable them to prop up heavy objects with loads exceeding 10,000 times their own weight. Also, the protein/CNTS hybrid achieves an ultrastiffness (over 10 MPa) and superelastic shape recovery (recovery strain >90%). Both experimental and numerical results indicate that the secondary conformational transition of silk fibroin plays a key role, where more α-helices/random coils transform into β-sheets under both confinement and low pressure. Our work reports a conformational transition mechanism of silk fibroin in a confined space, which provides guidance for constructing protein-based biological smart materials with potential applications in textiles, medicine, architecture, and other research fields.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"37 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143915770","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}

{"title":"Broadband-Responsive Rubbery Stretchable Vertical-Structured Photodetectors Based on Rubbery Stretchable Transparent Conductors","authors":"Junmei Hu, Wei-Chen Gao, Yu-Dong Zhao, Ben Fan, Xiang Sun, Jing Qiao, Ying-Shi Guan, Quan Li","doi":"10.1021/acsnano.5c01015","DOIUrl":"https://doi.org/10.1021/acsnano.5c01015","url":null,"abstract":"A rubbery stretchable conductor with high conductivity and transparency is crucial for the development of rubbery stretchable vertical-structured photodetectors. However, the development of such a rubbery conductor is still nascent. Here, we report the scalable manufacturing of rubbery stretchable transparent conductors (RSTCs) and the development of a rubbery stretchable vertical-structured photodetector (RSVPD). The RSTC is fabricated into a specialized micromesh structure by utilizing a close-packed monolayer of polystyrene microspheres as a mask. The micromesh structure not only enhances the conductor’s stretchability and transparency but also maintains its conductivity, making it ideal for various applications in stretchable electronics. The RSTCs are used to construct RSVPDs that have high response over a broad spectrum, and their electrical performances can be retained even when subjected to mechanical strains of up to 50%. Furthermore, a stretchable imager based on RSVPD was developed to detect the multipoint light distribution. Lastly, a photoplethysmography (PPG) sensor was also developed for real-time health monitoring.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"50 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143910778","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}