{"title":"Target-Zippable Anisotropic Near-Infrared AuNRs for Highly Reliable and Bright SERS Imaging of miRNA In Vivo","authors":"Yutian Lei, Chusheng Liu, Yakun Shi, Ping Li, Yanfei Zhang, Si-Yang Liu, Xing Han, Jiuxin Qu, Jianhe Guo, Zong Dai","doi":"10.1021/acs.nanolett.5c01375","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c01375","url":null,"abstract":"Near-infrared surface-enhanced Raman scattering (NIR-SERS) probes are promising for <i>in vivo</i> molecular imaging, but they face challenges in balancing plasmonic activity and signal reproducibility. We designed target-zippable anisotropic NIR gold nanorod (ani-NIR-AuNR) SERS probes, whose end and side regions are decorated with catalytic hairpin assembly (CHA) DNA hairpins and Raman reporters, respectively. These ani-NIR-AuNR monomers maintain a near-zero background until triggered by targets to form uniform side-by-side dimers with an average gap of 0.88 nm, synergistically amplifying electromagnetic enhancement and chemical enhancement. The CHA allows one target to zip numerous dimers, boosting hotspot density. These effects endow the SERS probes with good reproducibility (RSD = 8.56%), superior sensitivity (LOD = 0.15 fM), and a broad linear range (1 fM to 1 nM) for let-7d detection. Compared to fluorescence probes, they offer higher brightness, better spatial resolution, and longer signal persistence in <i>in vivo</i> miRNA imaging, demonstrating substantial potential in bioapplications.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"53 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876376","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":"Synchronous Regulation of S-Deficient ZnS-MoS2 Heterostructure Nanoreactor for Fast and Durable Sodium Storage","authors":"Ying Jiang, Mingyu Lian, Jinlian Ma, Yunsong Long, Xuejing Guo, Yitong Sun, Junchao Lao, Zhengqing Ye","doi":"10.1021/acs.nanolett.4c05957","DOIUrl":"https://doi.org/10.1021/acs.nanolett.4c05957","url":null,"abstract":"The enhancement of charge transfer and the relief of volume stress of anode materials contribute to fully exploiting electrochemical performance for sodium ion storage. Herein, a hollow carbon polyhedra nanoreactor adhered with a ZnS-MoS<sub>2</sub> heterostructure with tunable sulfur vacancy content (denoted as <i>hp</i>-ZMS-600/700/800) is prepared by self-assembly and a temperature dependent sulfurization procedure. The intimate heterointerface and moderate sulfur vacancies provide fast ion/electron transfer channels, and the hollow nanoreactors afford large volume variation and maintain structural integrity during the sodiation/desodiation process. Theoretical calculations and in situ/ex situ characterization techniques reveal both excellent electron/ion diffusion dynamics and a sodium storage mechanism. As a result, the optimized <i>hp</i>-ZMS-700 anode in sodium-ion batteries delivers a high initial Coulombic efficiency of 96.3%, a high capacity of 398 mAh g<sup>–1</sup> at 0.1 A g<sup>–1</sup>, good rate capability of 119.8 mAh g<sup>–1</sup> at 5 A g<sup>–1</sup>, and an excellent capacity retention of 84.6% after 1000 cycles at 2 A g<sup>–1</sup>.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"14 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876375","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}
Nano LettersPub Date : 2025-04-25DOI: 10.1021/acs.nanolett.5c01602
Qing Zhang, Yixuan Hu, Tao Yang, Han Chen, Yuto Ito, Daisuke Egusa, Eiji Abe, Qiwei Shi, Gang Ji, Yuchi Cui, Xiaodong Wang, Zhe Chen
{"title":"Chemical Short-Range Ordering in Nanoprecipitates Modulates Planar Faults to Enhance Mechanical Properties","authors":"Qing Zhang, Yixuan Hu, Tao Yang, Han Chen, Yuto Ito, Daisuke Egusa, Eiji Abe, Qiwei Shi, Gang Ji, Yuchi Cui, Xiaodong Wang, Zhe Chen","doi":"10.1021/acs.nanolett.5c01602","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c01602","url":null,"abstract":"Nanoprecipitates strengthen metallic materials by impeding dislocation motion, but they often compromise ductility. This study introduces a novel strategy to address this challenge by incorporating atomic-scale chemical heterogeneity within nanoprecipitates. For the first time, pronounced short-range ordering (SRO) within L1<sub>2</sub>-ordered precipitates of the Co<sub>40</sub>Ni<sub>30</sub>Cr<sub>20</sub>Al<sub>5</sub>Ti<sub>4</sub>Ta<sub>1</sub> multi-principal element alloy is observed and confirmed, with its formation mechanism elucidated via density functional theory. Experimental and computational results show that the unique atomic configuration reshapes the energy landscape of planar defects, enhancing the strength and work-hardening capacity. The SRO structure elevates the critical shear stress for dislocation-mediated precipitate shearing while reducing the formation energy of superlattice intrinsic stacking faults, thereby promoting nucleation site formation. This work pioneers a method for modulating atomic-scale heterogeneity within ordered structures, advancing high-performance material design.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"7 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876379","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}
Nano LettersPub Date : 2025-04-24DOI: 10.1021/acs.nanolett.5c01586
Jun Cai, Benyamin Shahryari, Alireza Seyedkanani, Agus P. Sasmito, Abdolhamid Akbarzadeh
{"title":"Topology-Dependent Enhancement of Pyroelectric Property in Nanoarchitected GaN Metamaterials","authors":"Jun Cai, Benyamin Shahryari, Alireza Seyedkanani, Agus P. Sasmito, Abdolhamid Akbarzadeh","doi":"10.1021/acs.nanolett.5c01586","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c01586","url":null,"abstract":"Pyroelectric materials exhibit spontaneous polarization in response to temperature fluctuations, a phenomenon known as the <i>pyroelectric effect</i>. This study investigates the pyroelectric properties of nanoarchitected gallium nitride (GaN) metamaterials with distinctive topologies, i.e., body-centered cube, octet truss, gyroid, and spinodoid, using molecular dynamics simulations. Our findings reveal a topology-dependent enhancement in the pyroelectric coefficient, primarily affected by the piezoelectric stress constant and thermal expansion coefficient. We demonstrate that decreasing the relative density further enhances the pyroelectric coefficient due to an increased surface-to-volume ratio that enhances the surface effects. Finally, we compute the pyroelectric figures of merit for thermal energy harvesting application, highlighting the superior pyroelectric performance of nanoarchitected GaN metamaterials compared to bulk GaN and GaN nanowires. These results underscore the potential of nanoscale topology engineering in the field of pyroelectricity for realizing next-generation nanogenerators, thermal imaging devices, and self-powered nanosensors.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"1 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872557","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}
Nano LettersPub Date : 2025-04-24DOI: 10.1021/acs.nanolett.5c01125
Zehua Zhao, Yan Zhang, Huandi Zhang, Xiaowei Shi, Haitao Zhao, Junpeng Liu, Jiamei Liu, Lei Li
{"title":"Gradient Structured Separator Enables Stable Aqueous Zinc Metal Batteries","authors":"Zehua Zhao, Yan Zhang, Huandi Zhang, Xiaowei Shi, Haitao Zhao, Junpeng Liu, Jiamei Liu, Lei Li","doi":"10.1021/acs.nanolett.5c01125","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c01125","url":null,"abstract":"Developing a functional separator is an important strategy to improve the electrochemical performance of the Zn anode by suppressing the Zn dendrite growth and parasitic side reactions, thus advancing the aqueous zinc-ion batteries. Herein, we experimentally realize functional separator with gradient-structure based on CeF<sub>3</sub> nanoparticles functionalized glass fibers. The experimental and theoretical results confirmed that the functional separator can tailor the Zn<sup>2+</sup> flux and restrain SO<sub>4</sub><sup>2–</sup> transport, promoting dense Zn deposition. The strong interaction between CeF<sub>3</sub> nanoparticles and H<sub>2</sub>O separates Zn<sup>2+</sup> and H<sub>2</sub>O at the electrolyte/Zn anode interface, suppressing side reactions. Consequently, the Zn||Zn with this separator achieves excellent cycling stability of 2500 h at 1 mA cm<sup>–2</sup> and 1 mAh cm<sup>–2</sup> and 1000 h at 5 mA cm<sup>–2</sup> and 5 mAh cm<sup>–2</sup>. This design of a functionalized separator provides a distinctive solution for the development of aqueous zinc-ion batteries.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"33 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872556","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":"In Situ Multiscale Study of Iron Oxidation at High Temperatures","authors":"Wei Tu, Zhen Zeng, Yongjian Zhao, Zhenghao Jia, Caixia Meng, Wei Liu, Xianhu Sun, Jianyu Huang","doi":"10.1021/acs.nanolett.5c00025","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c00025","url":null,"abstract":"Although high-temperature oxidation of metals results in significant failure of structure materials, in situ understanding of these processes and developing improved strategies are still very limited. Herein, using environmental scanning electron microscopy (ESEM), environmental transmission electron microscopy (ETEM), and X-ray photoelectron spectroscopy (XPS), we report the in situ dynamic high-temperature oxidation behaviors of iron in O<sub>2</sub>, H<sub>2</sub>O, and O<sub>2</sub> + H<sub>2</sub>O atmospheres, respectively. The results demonstrate that an oxygen-rich environment (1.6 mbar) leads to transient formation of polycrystalline Fe<sub>3</sub>O<sub>4</sub> without passivation effects on further oxidation, while sparse oxygen environments (10<sup>–3</sup> mbar) promote formation of a uniform thin passivation layer of Fe<sub>3</sub>O<sub>4</sub>, protecting itself from further oxidation in ambient air. In contrast to O<sub>2</sub>, the H<sub>2</sub>O vapor accelerates oxidation, and the products consist of Fe<sub>3</sub>O<sub>4</sub> and FeOOH. These in situ results give insights into designing technically universal antioxidation strategies.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"26 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143867253","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":"Highly Sensitive Wearable Chromic Force Sensor Utilizing In-Plane Anisotropy in Polydiacetylene Mechanochromism","authors":"Jianlu Zheng, Jiali Chen, Massimiliano Galluzzi, Yuge Hou, Kaori Sugihara","doi":"10.1021/acs.nanolett.5c00085","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c00085","url":null,"abstract":"Force sensitivity is a crucial parameter in mechanochromic materials, determining their application range and practical success. In this study, we reveal an unexplored degree of freedom─in-plane anisotropy─for significantly enhancing the force sensitivity of polydiacetylene. Utilizing our newly developed dual nanofriction force/fluorescence microscopy setup, we discovered that force sensitivity reaches its peak when external forces are applied perpendicular to the polymer backbones in-plane. This phenomenon is explained by a “domino effect”, where point loads propagate along the backbones and affect the polymer structure even hundreds of nanometers from the contact point. Leveraging this finding, we developed a highly sensitive, stretchable force sensor and demonstrated that aligning polydiacetylene crystals perpendicular to the force direction increased the sensor’s sensitivity by up to 14-fold.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"5 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143867256","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":"Collective Electricity Generation over the Kilovolt Level from Water Droplets","authors":"Wei Deng, Yufeng Zhu, Kelan Zhang, Yuxuan Yuan, Tao Hu, Xiao Wang, Jidong Li, Xuemei Li, Zhuhua Zhang, Wanlin Guo, Jun Yin","doi":"10.1021/acs.nanolett.5c01064","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c01064","url":null,"abstract":"Collective behavior enables groups of organisms to achieve feats far exceeding individual capability. Inspired by this, we present a novel droplet-based electricity generator that leverages the collective dynamics of multiple water droplets to significantly enhance electrical output, achieving orders of magnitude improvement compared with single-droplet devices. It is revealed that grouped water droplets, although spatially separated, coordinate via charge exchange with a solid surface and external charge transfer. Consequently, the solid surface charge density is significantly enhanced, elevating the charge transfer. This collective effect readily generates peak voltages exceeding one kilovolt, sufficient for air ionization and nitrogen fixation, with potential applications in nutrient production. We anticipate that this collective strategy will significantly advance the design and applications of droplet-based hydrovoltaic devices.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"130 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872555","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":"Keto-Oxygen on Graphitic Surface with Downshifted p-Band Center Achieves Efficient Metal-Free Transfer Hydrogenation of Nitroarenes","authors":"Rongjian Ding, Ting Zhang, Yanling Zhai, Haijie Cao, Zhijun Zhu, Xiaoquan Lu","doi":"10.1021/acs.nanolett.5c01614","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c01614","url":null,"abstract":"The critical challenge in utilizing carbon-based nanomaterials is identifying the active site. Herein, we demonstrate the keto-oxygen on the graphitic surface as active sites for catalytic transfer hydrogenation (CTH) and present an efficient nanocrystalline diamond (ND)-derived carbon-based catalyst for metal-free CTH of nitroarenes to imine with 99.9% nitrobenzene conversion and exclusive selectivity (99.9%). By selectively deconstructing the graphitic surface or eliminating carbonyl groups, the graphite-conjugated carbonyl group is confirmed as the catalytically active site. Moreover, kinetic studies display the lower activation barrier of benzylalcohol than that of nitrobenzene (88.8 vs 119.1 kJ mol<sup>–1</sup>, respectively), indicating that alcohol dehydrogenation occurs prior to the activation of nitrobenzene. Density functional theory calculations reveal the downshifted <i>p</i>-band center of keto-oxygen on the <i>sp</i><sup>2</sup> hybrid C surface affords moderate adsorption of benzaldehyde intermediates, which accelerates the formation of active H for the following hydrogenation step and is responsible for the high catalytic activity.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"7 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872558","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}
Nano LettersPub Date : 2025-04-24DOI: 10.1021/acs.nanolett.5c01242
Shiying Shen, Haoran Lu, Shriya Gumber, Oleg V. Prezhdo, Run Long
{"title":"Interplay of Ultrafast Electron–Phonon and Electron–Electron Scattering in Ti3C2Tx MXenes: Ab Initio Quantum Dynamics","authors":"Shiying Shen, Haoran Lu, Shriya Gumber, Oleg V. Prezhdo, Run Long","doi":"10.1021/acs.nanolett.5c01242","DOIUrl":"https://doi.org/10.1021/acs.nanolett.5c01242","url":null,"abstract":"Nonthermal electrons are vital in solar energy and optoelectronics, yet their relaxation pathways are not fully understood. Ab initio quantum dynamics reveal that in Ti<sub>3</sub>C<sub>2</sub>O<sub>2</sub> electron–phonon (e-ph) relaxation is faster than electron–electron (e-e) scattering due to strong coupling with the A<sub>1g</sub> phonon at 190 cm<sup>–1</sup> and the presence of light C and O atoms. Nuclear quantum effects are minimal; vibrations influence e-e scattering only indirectly, and the A<sub>1g</sub> mode’ zero-point energy is much lower than thermal energy at ambient conditions. Substituting O with heavier S in Ti<sub>3</sub>C<sub>2</sub>OS slows e-ph relaxation and enhances e-e scattering, making it a faster process. However, both channels proceed concurrently, challenging the e-e and e-ph time scale separation often used for metals. These results underscore the need for atomistic-level understanding of nonthermal electron dynamics, especially in light-element systems such as MXenes, and provide guidance for optimizing electronic relaxation in advanced optoelectronic materials and devices.","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":"97 1","pages":""},"PeriodicalIF":10.8,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872721","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}